scholarly journals Comparison of surface ozone simulation among selected regional models in MICS-Asia III – effects of chemistry and vertical transport for the causes of difference

2019 ◽  
Vol 19 (1) ◽  
pp. 603-615 ◽  
Author(s):  
Hajime Akimoto ◽  
Tatsuya Nagashima ◽  
Jie Li ◽  
Joshua S. Fu ◽  
Dongsheng Ji ◽  
...  

Abstract. In order to clarify the causes of variability among the model outputs for surface ozone in the Model Intercomparison Study Asia Phase III (MICS-Asia III), three regional models, CMAQ v.5.0.2, CMAQ v.4.7.1, and NAQPMS (abbreviated as NAQM in this paper), have been selected. Detailed analyses of monthly averaged diurnal variation have been performed for selected grids covering the metropolitan areas of Beijing and Tokyo and at a remote oceanic site, Oki. The chemical reaction mechanism, SAPRC99, used in the CMAQ models tended to give a higher net chemical ozone production than CBM-Z used in NAQM, agreeing with previous studies. Inclusion of the heterogeneous “renoxification” reaction of HNO3 (on soot surface)→NO+NO2 only in NAQM would give a higher NO concentration resulting in a better agreement with observational data for NO and nighttime O3 mixing ratios. In addition to chemical processes, the difference in the vertical transport of O3 was found to affect the simulated results significantly. Particularly, the increase in downward O3 flux from the upper layer to the surface after dawn was found to be substantially different among the models. Larger early morning vertical transport of O3 simulated by CMAQ 5.0.2 is thought to be the reason for higher daytime O3 in July in this model. All three models overestimated the daytime ozone by ca. 20 ppbv at the remote site Oki in July, where in situ photochemical activity is minimal.

2018 ◽  
Author(s):  
Hajime Akimoto ◽  
Tatsuya Nagashima ◽  
Jie Li ◽  
Joshua Fu ◽  
Dongsheng Ji ◽  
...  

Abstract. In order to clarify the cause of variability among the model outputs for surface ozone in the Model Intercomparison Study Asia Phase III (MICS-Asia III), three regional models, CMAQ v.5.0.2, CMAQ v.4.7.1 and NAQPMS (abbreviated as NAQM in this paper) have been selected. The detailed analyses have been made for monthly averaged diurnal variation for select grids covering metropolitan area of Beijing and Tokyo, and at a remote oceanic site, Oki. The chemical reaction mechanism, SAPRC99 used in the CMAQ models tends to give higher net chemical ozone production than CBM-Z used in NAQM agreeing with previous studies. Inclusion of heterogeneous “renoxification” reaction of HNO3 (on soot) → NO + NO2 only in NAQM is supposed to give higher NO concentration to give better agreement with observational data for NO and nighttime O3 mixing ratios. In addition to chemistry, the difference in vertical transport of O3 was found to affect the simulated results significantly. Particularly, the increase in downward flux of O3 from upper layer to the surface after the dawn is found to be substantially different among the models. Larger early morning vertical transport of O3 by CMAQ 5.0.2 would be the reason for higher daytime O3 by this model in July. All the three models overestimate the daytime ozone by ca. 20 ppbv at the remote site Oki in July, where in situ photochemical activity is minimal.


2016 ◽  
Author(s):  
Imran A. Girach ◽  
Narendra Ojha ◽  
Prabha R. Nair ◽  
Andrea Pozzer ◽  
Yogesh K. Tiwari ◽  
...  

Abstract. We present ship-borne measurements of surface ozone, carbon monoxide and methane over the Bay of Bengal (BoB), the first time such measurements have been taken during the summer monsoon season, as a part of the Continental Tropical Convergence Zone (CTCZ) experiment during 2009. O3, CO, and CH4 mixing ratios exhibited significant spatial and temporal variability in the ranges of 8–54 nmol mol−1, 50–200 nmol mol−1, and 1.57–2.15 µmol mol−1, with means of 29.7 ± 6.8 nmol mol−1, 96 ± 25 nmol mol−1, and 1.83 ± 0.14 µmol mol−1, respectively. The average mixing ratios of trace gases over northern BoB (O3: 30 ± 7 nmol mol−1, CO: 95 ± 25 nmol mol−1, CH4: 1.86 ± 0.12 µmol mol−1), in airmasses from northern or central India, did not differ much from those over central BoB (O3: 27 ± 5 nmol mol−1, CO: 101 ± 27 nmol mol−1, CH4: 1.72 ± 0.14 µmol mol−1), in airmasses from southern India. Spatial variability is observed to be most significant for CH4. The ship-based observations, in conjunction with backward air trajectories and ground-based measurements over the Indian region, are analyzed to estimate a net ozone production of 1.5–4 nmol mol−1 day−1 in the outflow. Ozone mixing ratios over the BoB showed large reductions (by ~ 20 nmol mol−1) during four rainfall events. Temporal changes in the meteorological parameters, in conjunction with ozone vertical profiles, indicate that these low ozone events are associated with downdrafts of free-tropospheric ozone-poor airmasses. While the observed variations in O3 and CO are successfully reproduced using the Weather Research and Forecasting model with Chemistry (WRF-Chem), this model overestimates mean concentrations by about 20 %, generally overestimating O3 mixing ratios during the rainfall events. Analysis of the chemical tendencies from model simulations for a low-O3 event on August 10, 2009, captured successfully by the model, shows the key role of horizontal advection in rapidly transporting ozone-rich airmasses across the BoB. Our study fills a gap in the availability of trace gas measurements over the BoB, and when combined with data from previous campaigns, reveals large seasonal amplitude (~ 39 and ~ 207 nmol mol−1 for O3 and CO, respectively) over the northern BoB.


2017 ◽  
Author(s):  
Xiufeng Yin ◽  
Shichang Kang ◽  
Benjamin de Foy ◽  
Zhiyuan Cong ◽  
Jiali Luo ◽  
...  

Abstract. Ozone is an important pollutant and greenhouse gas, and tropospheric ozone variations are generally associated with both natural and anthropogenic processes. As one of the most pristine and inaccessible regions in the world, the Tibetan Plateau has been considered as an ideal region for studying processes of the background atmosphere. Due to the vast area of the Tibetan Plateau, sites in the southern, northern and central regions exhibit different patterns of variation in surface ozone. Here, we present long-term measurements for ~ 5 years (January 2011 to October 2015) of surface ozone mixing ratios at Nam Co Station, which is a regional background site in the inland Tibetan Plateau. An average surface ozone mixing ratio of 47.6 ± 11.6 ppb was recorded, and a large annual cycle was observed with maximum ozone mixing ratios in the spring and minimum ratios during the winter. The diurnal cycle is characterized by a minimum in the early morning and a maximum in the late afternoon. Nam Co Station represents a background region where surface ozone receives negligible local anthropogenic emissions. Surface ozone at Nam Co Station is mainly dominated by natural processes involving photochemical reactions and potential local vertical mixing. Model results indicate that the study site is affected by the surrounding areas in different seasons and that air masses from the northern Tibetan Plateau lead to increased ozone levels in the summer. In contrast to the surface ozone levels at the edges of the Tibetan Plateau, those at Nam Co Station are less affected by stratospheric intrusions and human activities which makes Nam Co Station representative of vast background areas in the central Tibetan Plateau. By comparing measurements at Nam Co Station with those from other sites in the Tibetan Plateau and beyond, we aim to expand the understanding of ozone cycles and transport processes over the Tibetan Plateau. This work may provide a reference for model simulations in the future.


2008 ◽  
Vol 8 (2) ◽  
pp. 5359-5412 ◽  
Author(s):  
P. M. Sheehy ◽  
R. Volkamer ◽  
L. T. Molina ◽  
M. J. Molina

Abstract. A box model using measurements from the Mexico City Metropolitan Area study in the spring of 2003 (MCMA-2003) is presented to study ROx (ROx=OH+HO2+RO2+RO) radical cycling in the troposphere. Model simulations were performed with the Master Chemical Mechanism (MCMv3.1) constrained with 10 min averaged measurements of major radical sources (i.e., HCHO, HONO, O3, CHOCHO, etc.), radical sink precursors (i.e., NO, NO2, SO2, CO, and 102 volatile organic compounds VOC), meteorological parameters (temperature, pressure, water vapor concentration, dilution), and photolysis frequencies. Modeled HOx concentrations compare favorably with measured concentrations for most of the day; however, the model under-predicts the concentrations of radicals in the early morning. This "missing reactivity" is highest during peak photochemical activity, and is least visible in a direct comparison of HOx radical concentrations. The true uncertainty due to "missing reactivity" is apparent in parameters like chain length, and ozone production (P(O3)). For example, the integral amount of ozone produced could be under-predicted by a factor of two. Our analysis highlights that apart from uncertainties in emissions, and meteorology, there is an additional major chemical uncertainty in current models.


2018 ◽  
Vol 18 (3) ◽  
pp. 2175-2198 ◽  
Author(s):  
Emmanouil Oikonomakis ◽  
Sebnem Aksoyoglu ◽  
Giancarlo Ciarelli ◽  
Urs Baltensperger ◽  
André Stephan Henry Prévôt

Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (< 40 ppb) by 5–15 ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone–temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, four scenarios were tested: (i) increased volatile organic compound (VOC) emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased nitrogen oxide (NOx) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased traffic-only NOx emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NOx emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone–temperature correlation is also better when NOx emissions are doubled. In the Benelux area, however, the third scenario (where both NOx and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NOx emissions by a factor of 4 gave very similar results to the doubling of all NOx emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NOx emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 ∘C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NOx) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.


2017 ◽  
Author(s):  
Emmanouil Oikonomakis ◽  
Sebnem Aksoyoglu ◽  
Giancarlo Ciarelli ◽  
Urs Baltensperger ◽  
André S. H. Prévôt

Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modelling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, CAMx. The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (


2011 ◽  
Vol 11 (5) ◽  
pp. 15975-16021 ◽  
Author(s):  
C. Buizert ◽  
P. Martinerie ◽  
V. V. Petrenko ◽  
J. P. Severinghaus ◽  
C. M. Trudinger ◽  
...  

Abstract. Compacted snow (firn) preserves a continuous record of atmospheric composition up to a century back in time. Firn air transport modeling is essential for interpretation of firn gas records. Each site needs to be characterised individually through a tuning procedure, in which the effective diffusivity at each depth is adjusted to optimise the agreement between modeled and measured mixing ratios of a selected reference gas (usually CO2). We present the characterisation of the NEEM site, Northern Greenland (77.45° N 51.06° W), where an ensemble of ten reference tracers is used to constrain the diffusivity reconstruction. By analysing uncertainties in both data and the reference gas atmospheric histories, we can objectively assign weights to each of the gases used for the model tuning, and define a root mean square criterion that is minimised in the tuning. Each tracer constrains the firn profile differently through its unique atmospheric history and free air diffusivity, making our multiple-tracer characterisation method a clear improvement over the commonly used single-tracer tuning. Six firn air transport models are tuned to the NEEM site; all models successfully reproduce the data within a 1σ Gaussian distribution. The modern day Δage, i.e. the difference between gas age and ice age, is calculated to be 182 ± 8 yr. We find evidence that diffusivity does not vanish completely in the firn lock-in zone, as is commonly assumed. We further present the first intercomparison study of firn air models, where we introduce diagnostic scenarios designed to probe specific aspects of the model physics. Our results show that there are major differences in the way the models handle advective transport. Furthermore diffusive fractionation of isotopes in the firn is poorly constrained by the models, which has consequences for attempts to reconstruct the isotopic composition of trace gases back in time using firn air and ice core records.


2021 ◽  
Vol 14 (10) ◽  
pp. 6155-6175
Author(s):  
Mingshuai Zhang ◽  
Chun Zhao ◽  
Yuhan Yang ◽  
Qiuyan Du ◽  
Yonglin Shen ◽  
...  

Abstract. Biogenic volatile organic compounds (BVOCs) simulated by current air quality and climate models still have large uncertainties, which can influence atmospheric chemistry and secondary pollutant formation. These modeling sensitivities are primarily due to two sources. One originates from different treatments in the physical and chemical processes associated with the emission rates of BVOCs. The other is errors in the specification of vegetation types and their distribution over a specific region. In this study, the version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) updated by the University of Science and Technology of China (USTC version of WRF-Chem) from the public WRF-Chem(v3.6) is used. The modeling results over eastern China with different versions (v1.0, v2.0, v3.0) of the Model of Emissions of Gases and Aerosols from Nature (MEGAN) in WRF-Chem are examined or documented. Sensitivity experiments with these three versions of MEGAN and two vegetation datasets are conducted to investigate the difference of three MEGAN versions in modeling BVOCs and its dependence on the vegetation distributions. The experiments are also conducted for spring (April) and summer (July) to examine the seasonality of the modeling results. The results indicate that MEGAN v3.0 simulates the largest amount of biogenic isoprene emissions over eastern China. The different performance among MEGAN versions is primarily due to their different treatments of applying emission factors and vegetation types. In particular, the results highlight the importance of considering the sub-grid vegetation fraction in estimating BVOC emissions over eastern China, which has a large area of urbanization. Among all activity factors, the temperature-dependent factor dominates the seasonal change of activity factor in all three versions of MEGAN, while the different response to the leaf area index (LAI) change determines the difference among the three versions in seasonal variation of BVOC emissions. The simulated surface ozone concentration due to BVOCs can be significantly different (ranging from 1 to more than 10 ppbv in some regions) among the experiments with three versions of MEGAN, which is mainly due to their impacts on surface VOCs and NOx concentrations. Theoretically MEGAN v3.0 that is coupled with the land surface scheme and considers the sub-grid vegetation effect should overcome previous versions of MEGAN in WRF-Chem. However, considering uncertainties of retrievals and anthropogenic emissions over eastern China, it is still difficult to apply satellite retrievals of formaldehyde and/or limited sparse in situ observations to constrain the uncertain parameters or functions in BVOC emission schemes and their impacts on photochemistry and ozone production. More accurate vegetation distribution and measurements of biogenic emission fluxes and species concentrations are still needed to better evaluate and optimize models.


2021 ◽  
Author(s):  
Mingshuai Zhang ◽  
Chun Zhao ◽  
Yuhan Yang ◽  
Qiuyan Du ◽  
Yonglin Shen ◽  
...  

Abstract. Biogenic volatile organic compounds (BVOCs) simulated by current air quality and climate models still have large uncertainties, which can influence atmosphere chemistry and secondary pollutant formation over East China. These uncertainties are generally resulted from two sources. One is from different biogenic emission schemes coupled in model, representing for different treatments of physical and chemistry progresses during the emissions of BVOCs. The other is from the biased distribution of vegetation types over a specific region. In this study, the version of WRF-Chem updated by the University of Science and Technology of China (USTC version of WRF-Chem) from the public WRF-Chem(v3.6) is used. The modeling results over East China with different versions (v1.0, v2.0, v3.0) of Model of Emissions of Gases and Aerosols from Nature (MEGAN) in WRF-Chem are examined and documented. Sensitivity experiments with these three versions of MEGAN and two vegetation datasets are conducted to investigate the difference of three MEGAN versions in modeling biogenic VOCs and its dependence on the vegetation distributions. The experiments are also conducted for spring (April) and summer (July) to examine the seasonality of the modeling results. The results indicate that MEGANv3.0 simulates the largest amount of biogenic isoprene emissions over East China. The different performance among MEGAN versions is primarily due to their different treatments of applying emission factors and vegetation types. In particular, the results highlight the importance of considering sub-grid vegetation fraction in estimating BVOCs emissions. Among all activity factors, temperature-dependent factor dominates the seasonal change of activity factor in all three versions of MEGAN, while the different response to the leaf area index (LAI) change determines the difference among the three versions in seasonal variation of BVOC emissions. The simulated surface ozone concentration due to BVOCs can be significantly different among the experiments with three versions of MEGAN, which is mainly due to their impacts on surface VOCs and NOx concentrations. This study suggests that there is still large uncertain range in modeling BVOCs and their impacts on photochemistry and ozone production. More accurate vegetation distribution and measurements of biogenic emission flux and species concentration are needed to evaluate the model performance and reduce the uncertainties.


2017 ◽  
Vol 17 (11) ◽  
pp. 7127-7142 ◽  
Author(s):  
Yudong Yang ◽  
Min Shao ◽  
Stephan Keßel ◽  
Yue Li ◽  
Keding Lu ◽  
...  

Abstract. Total OH reactivity measurements were conducted on the Peking University campus (Beijing) in August 2013 and in Heshan (Guangdong province) from October to November 2014. The daily median OH reactivity was 20 ± 11 s−1 in Beijing and 31 ± 20 s−1 in Heshan, respectively. The data in Beijing showed a distinct diurnal pattern with the maxima over 27 s−1 in the early morning and minima below 16 s−1 in the afternoon. The diurnal pattern in Heshan was not as evident as in Beijing. Missing reactivity, defined as the difference between measured and calculated OH reactivity, was observed at both sites, with 21 % missing reactivity in Beijing and 32 % missing reactivity in Heshan. Unmeasured primary species, such as branched alkenes, could contribute to missing reactivity in Beijing, especially during morning rush hours. An observation-based model with the RACM2 (Regional Atmospheric Chemical Mechanism version 2) was used to understand the daytime missing reactivity in Beijing by adding unmeasured oxygenated volatile organic compounds and simulated intermediates of the degradation from primary volatile organic compounds (VOCs). However, the model could not find a convincing explanation for the missing reactivity in Heshan, where the ambient air was found to be more aged, and the missing reactivity was presumably attributed to oxidized species, such as unmeasured aldehydes, acids and dicarbonyls. The ozone production efficiency was 21 % higher in Beijing and 30 % higher in Heshan when the model was constrained by the measured reactivity, compared to the calculations with measured and modeled species included, indicating the importance of quantifying the OH reactivity for better understanding ozone chemistry.


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