The Interannual Variation of Transboundary Contributions from Chinese Emissions of PM_(2.5)to South Korea

In recent years,several studies pointed out that anthropogenic emission sources in China which significantly contribute to the PM_(2.5)mass burden was an important cause of particulate pollution in South Korea.However,most studies generally focused upon a single pollution event.It is rare to see comprehensive research that captures those features prone to interannual variations concerning the transboundary pollutant contribution in South Korea using a unified method.In this paper,we establish the emission inventories covering East Asia in 2010,2015,and 2017,and then conduct the source apportionment by applying a coupled regional air quality model called the Integrated Source Apportionment Module(ISAM).Comparison of simulated and observed PM_(2.5)mass concentration at 165 CNEMC(China National Environmental Monitoring Center)sites suggests that the PM_(2.5)concentrations are well represented by the modeling system.The model is used to quantitatively investigate the contribution from emission sources in China to PM_(2.5)concentrations over South Korea and those features found to be prone to interannual variations are then discussed.The results show that the average annual contribution of PM_(2.5)has dropped significantly from 28.0%in 2010 to 15.7%in 2017,which strongly suggests that China has achieved remarkable results in the treatment of atmospheric particulates.

Visco-acoustic transmission waveform inversion of velocity structure in space-frequency domain

According to the least square criterion of minimizing the misfit between modeled and observed data, this paper provides a preconditioned gradient method to invert the visco-acoustic velocity structure on the basis of using sparse matrix LU factorization technique to directly solve the visco-acoustic wave forward problem in space-frequency domain. Numerical results obtained in an inclusion model inversion and a layered homogeneous model inversion demonstrate that different scale media have their own frequency responses, and the strategy of using low-frequency inverted result as the starting model in the high-frequency inversion can greatly reduce the non-tmiqueness of their solutions. It can also be observed in the experiments that the fast convergence of the algorithm can be achieved by using diagonal elements of Hessian matrix as the preconditioned operator, which fully incorporates the advantage of quadratic convergence of Gauss-Newton method.

Impacts of the meteorological condition versus emissions reduction on the PM_(2.5) concentration over Beijing-Tianjin-Hebei during the COVID-19 lockdown

本研究从气象条件和减排两方面探讨了COVID-19封锁期间严重雾霾发生的原因[研究目的],并定量的分析了气象条件和减排对PM_(2.5)浓度的相对影响[创新点].使用WRF-Chem在2019年2月3日–16日和2020年2月3日–16日进行了三个数值模拟试验,分别为2019年气象场与MEIC-2019(2019年中国多分辨率月度排放清单),2020年气象场与MEIC-2019,2020年气象场与MEIC-2020[研究方法].结果表明COVID-19封锁期间严重雾霾的原因是不利气象条件增加的PM_(2.5)浓度大于减排减少的PM_(2.5)浓度[重要结论].

不同代表性浓度路径情景下2045-2050年中国气溶胶分布变化的分析

基于来自于CMIP5中CESM模式的三种RCP情景下的气象场的降尺度模拟,应用区域空气质量模式系统RAMSCMAQ模拟2045-2050年中国地区气溶胶浓度.三种RCP情景下气象场的降尺度模拟表明,与RCP2.6相比,在RCP4.5和RCP8.5下,华北和华南的近地表温度差减小,风速在华北和华南地区增加,在中部地区下降.RCP2.6情景下,模拟的2045年到2050年平均的PM_(2.5)浓度在华北平原,长三角的部分地区和四川盆地最高,约为40-50μg m^(-3),在中国中部和珠三角的部分地区约为30-40μg m^(-3).与RCP2.6相比,在RCP4.5和RCP8.5下,PM_(2.5)增加了4-12μg m^(-3),其中在RCP4.5和RCP8.5下,SO_(4)^(2-)和NH_(4+)的浓度增加,在RCP4.5下,NO^(3-)浓度降低,在RCP8.5下,NO^(3-)浓度升高,在RCP4.5和RCP8.5下,BC浓度变化很小,而OC浓度下降,其中在RCP8.5下,西南和东南部分地区的OC有所增加.不同的气溶胶物种浓度在RCP4.5和RCP2.6之间的差异以及RCP8.5和RCP2.6之间的差异具有相似的年度变化,这表明气候变化对不同物种的影响趋于一致.

Sensitivity analysis of surface ozone to emission controls in Beijing and its neighboring area during the 2008 Olympic Games

The regional air quality modeling system RAMS （Regional Atmospheric Modeling System）-CMAQ （Community Multi-scale Air Quality modeling system） is applied to analyze temporal and spatial variations in surface ozone concentration over Beijing and its surrounding region from July to October 2008.Comparison of simulated and observed meteorological elements and concentration of nitrogen oxides （NOx） and ozone at one urban site and three rural sites during Olympic Games show that model can generally reproduce the main observed feature of wind,temperature and ozone,but NOx concentration is overestimated.Although ozone concentration decreased during Olympics,high ozone episodes occurred on 24 July and 24 August with concentration of 360 and 245 μg/m 3 at Aoyuncun site,respectively.The analysis of sensitive test,with and without emission controls,shows that emission controls could reduce ozone concentration in the afternoon when ozone concentration was highest but increase it at night and in the morning.The evolution of the weather system during the ozone episodes （24 July and 24 August） indicates that hot and dry air and a stable weak pressure field intensified the production of ozone and allowed it to accumulate.Process analysis at the urban site and rural site shows that under favorable weather condition on 24 August,horizontal transport was the main contributor of the rural place and the pollution from the higher layer would be transported to the surface layer.On 24 July,as the wind velocity was smaller,the impact of transport on the rural place was not obvious.

Simulation of atmospheric aerosols in East Asia using modeling system RAMS-CMAQ:Model evaluation

The modeling system RAMS-CMAQ is applied in this paper to East Asia to simulate the temporo-spatial concentration distributions of atmospheric aerosols. For evaluating its performances, modeled concentrations of aerosols such as sulfate, nitrate, ammonium, black carbon and organic carbon were compared with observations obtained in East Asia on board of two aircrafts in the springtime of 2001. The comparison showed generally good agreement, and, in particular, that the modeling system captured most of the important observed features, including vertical gradients of the aerosols of the Asian outflow over the western Pacific. The evaluation results provide us with much confidence for further use of the modeling system to investigate the transport and transformation processes of atmospheric aerosols over East Asia and to assess their impacts on the Earth＇s radiation budget.

NUMERICAL SIMULATION WITH A COMPREHENSIVE CHEMICAL TRANSPORT MODEL OF NITRATE,SULFATE,AND AMMONIUM AEROSOL DISTRIBUTIONS OVER EAST ASIA

The transport and chemical production processes of nitrate, sulfate, and ammonium aerosols over East Asia were investigated by use of the Models-3 Community Multi-scale Air Quality （CMAQ） modeling system coupled with the Regional Atmospheric Modeling System （RAMS）. For the evaluation of the model＇s ability in depicting their 3-dimensional concentration distributions and temporal variations, modeled concentrations of nitrate, sulfate, and ammonium aerosols are compared with the observations obtained at a ground station in Japan in March 2001 and onboard of an aircraft DC-8 on 18 and 21 March 2001 during the Transport and Chemical Evolution over the Pacific （TRACE-P） field campaign. Comparison shows that simulated values of nitrate, sulfate, and ammonium aerosols are generally in good agreement with their observed data, and the model captures most important observed features, and reproduces temporal and spatial variations of nitrate, sulfate, and ammonium aerosol concentrations reasonably well, e.g., the timing and locations of the concentration spikes of nitrate, sulfate, and ammonium aerosols are well reproduced, but large discrepancies between observed and simulated values are also clearly seen at some points and some times due to the coarse grid resolution and uncertainties of the emissions used in this study. This comparison results indicate that CMAQ is able to simulate the distributions of nitrate, sulfate, and ammonium aerosols and their related species in the troposphere over East Asia reasonably well.

Accounting for CO2 Variability over East Asia with a Regional Joint Inversion System and Its Preliminary Evaluation

A regional surface carbon dioxide （C02） flux inversion system, the Tan-Tracker-Region, was developed by incor- porating an assimilation scheme into the Community Multiscale Air Quality （CMAQ） regional chemical transport model to resolve fine-scale CO2 variability over East Asia. The proper orthogonal decomposition-based ensemble four-dimensional variational data assimilation approach （POD-4DVar） is the core algorithm for the joint assimilation framework, and simultaneous assimilations of CO2 concentrations and surface CO2 fluxes are applied to help reduce the uncertainty in initial CO2 concentrations. A persistence dynamical model was developed to describe the evolu- tion of the surface CO2 fluxes and help avoid the ＂signal-to-noise＂ problem; thus, CO2 fluxes could be estimated as a whole at the model grid scale, with better use of observation information. The performance of the regional inversion system was evaluated through a group of single-observation-based observing system simulation experiments （OSSEs）. The results of the experiments suggest that a reliable performance of Tan-Tracker-Region is dependent on certain assimilation parameter choices, for example, an optimized window length of approximately 3 h, an ensemble size of approximately 100, and a covariance localization radius of approximately 320 km. This is probably due to the strong diurnal variation and spatial heterogeneity in the fine-scale CMAQ simulation, which could affect the perform- ance of the regional inversion system. In addition, because all observations can be artificially obtained in OSSEs, the performance of Tan-Tracker-Region was further evaluated through different densities of the artificial observation net- work in different CO2 flux situations. The results indicate that more observation sites would be useful to systematic- ally improve the estimation of CO2 concentration and flux in large areas over the model domain. The work presented here forms a foundation for future research in which a thorough estimation of CO2 flux variability over East Asia could be performed with the regional inversion system.

Local and long-range transport influences on PM_(2.5) at a cities-cluster in northern China,during summer 2008

Hourly PM2.5 concentrations were observed simultaneously at a cities-cluster comprising 10 cities/towns in Hebei province in China from July 1 to 31, 2008. Among the 10 cities/towns, Baoding showed the high- est average concentration level （161.57μg/m3） and Yanjiao exhibited the lowest （99.35 μg/m3 ）. These observed data were also studied using the joint potential source contribution function with 24-h and 72-h backward trajectories, to identify more clearly the local and countrywide-scale long-range transport sources. For the local sources, three important influential areas were found, whereas five important influential areas were defined for long-range transport sources. Spatial characteristics of PM2.5 were determined by multivariate statistical analyses. Soil dust, coal combustion, and vehicle emissions might be the potential contributors in these areas. The results of a hierarchical cluster analysis for back trajectory endpoints and PM2.s concentrations datasets show that the spatial characteristics of PM2.5 in the cities-cluster were influenced not only by local sources, but also by long-range transport sources. Different cities in the cities-cluster obtained different weighted contributions from local or long-range transport sources. Cangzhou, Shijiazhuang, and Baoding are near the source areas in the south of Hebei province, whereas Zhuozhou, Yangfang, Yanjiao, Xianghe, and Langfang are close to the sources areas near Beijing and Tianjin.

Development of CMAQ for East Asia CO_2 data assimilation under an EnKF framework: a first result

Under an Ensemble Kalman Filter(EnKF)framework,Regional Atmospheric Modeling System and Models-3 Community Multi-scale Air Quality(RAMS–CMAQ)modeling system is developed to be a CO2data assimilation system EnKF–CMAQ,and the EnKF–CMAQ system is then applied to East Asia for validation with real continuous surface CO2concentration observations available in the study domain instead of using an observation simulation system experiment.Experiments with an experimental period of January 23 to February 7,2007 are conducted,and the experimental results of the EnKF–CMAQ system and the RAMS–CMAQ model are compared against continuous surface CO2observations from assimilation sites and independent reference sites.Distributions of daily mean CO2concentration increments show that the EnKF–CMAQ system confines the update of daily mean CO2within areas nearby and downwind of the assimilation sites.Both the CO2concentration ensemble spreads and background error covariances show flow-dependent patterns.The results indicate the crucial role of wind transport in the CO2data assimilation,which agrees with the previous studies.The average bias and the average root-mean-square error(RMSE)of daily mean CO2concentration at the assimilation sites are reduced by 1.00 and1.83 ppm,respectively,and those at the reference sites are reduced by 0.24 and 0.22 ppm,respectively.The results demonstrate the EnKF–CMAQ system is capable of assimilating the continuous surface CO2concentration observations to improve the simulation accuracy of the atmospheric CO2synoptic variation.Since growing CO2observations over East Asia are being available nowadays,this work is our first step to generate consistent spatial and temporal atmospheric CO2concentration fields over East Asia,particularly over China,using both in situ and satellite observations.

Investigating missing sources of glyoxal over China using a regional air quality model (RAMS-CMAQ)

Currently, modeling studies tend to significantly underestimate observed space-based glyoxal （CHOCHO） vertical column densities （VCDs）, implying the existence of missing sources of giyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors. In case 1, where the emissions of aromatic compounds were increased three-fold, improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were B-B-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case B, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of giyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes （a two-fold increase）, the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July.

Modeling nitrate aerosol distributions and its direct radiative forcing in East Asia with RAMS-CMAQ

The geographical and seasonal characteristics in nitrate aerosol and its direct radiative forcing over East Asia are analyzed by using the air quality modeling system RAMS-CMAQ coupled with an aerosol optical properties/radiative transfer module. For evaluating the model performance, nitrate ion concentration in precipitation, and mixing ratios of PMl0, and some gas precursors of aerosol during the whole year of 2007 are compared against surface observations at 17 stations located in Japan, Korea, and China, and the satellite retrieved NO2 columns, The comparison shows that the simulated values are generally in good agreement with the observed ones. Simulated monthly averaged values are mostly within a factor of 2 of the measurements at the observation stations. The distribution patterns of NO2 from simulation and satellite measurement are also similar with each other. Analysis of the distribution features of monthly and yearly averaged mass concentration and direct radiative forcing （DRF） of nitrate indicates that the nitrate aerosol could reach about 25-30% of the total aerosol mass concentration and DRF in Sichuan Basin, Southeast China, and East China where the high mass burden of all major aerosols concentrated. The highest mass concentration and strongest DRF of nitrate could exceed 40 μg/m^3 and -5 Wire2, respectively. It also indicates that other aerosol species, such as carbonaceous and mineral particles, could obviously influence the nitrate DRF for they are often internally mixed with each other.

Modeling study on seasonal variation in aerosol extinction properties over China

To investigate the seasonal variation of aerosol optical depth （AOD）, extinction coefficient （EXT）, single scattering albedo （SSA） and the decomposed impacts from sulfate （SO42-） and black carbon （BC） over China, numerical experiments are conducted from November 2007 to December 2008 by using WRF-Chem. Comparison of model results with measurements shows that model can reproduce the spatial distribution and seasonal variation of AOD and SSA. Over south China, AOD is largest in spring （0.6-1.2） and lowest in summer （0.2-0.6）. Over north, northeast and east China, AOD is highest in summer while lowest in winter. The high value of EXT under 850 hPa which is the reflection of low visibility ranges from 0.4-0.8 km-1 and the high value area shifts to north during winter, spring and summer, then back to south in autumn. SSA is 0.92-0.94 in winter and 0.94-0.96 for the other three seasons because of highest BC concentration in winter over south China. Over east China, SSA is highest （0.92-0.96） in summer, and 0.88-0.92 during winter, spring and autumn as the concentration of scattering aerosol is highest while BC concentration is lowest in summer over this region. Over north China, SSA is highest （0.9-0.94） in summer and lowest （0.82-0.86） in winter due to the significant variation of aerosol concentration. The SOn2- induced EXT increases about 5%- 55% and the impacts of BC on EXT is much smaller （2%-10%）. The SO42--induced increase in SSA is 0.01-0.08 and the BC-induced SSA decreases 0.02-0.18.