Towards the improvements of simulating the chemical and optical properties of Chinese aerosols using an online coupled model – CUACE/Aero

ABSTRACT CUACE/Aero, the China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment for aerosols, is a comprehensive numerical aerosol module incorporating emissions, gaseous chemistry and size-segregated multi-component aerosol algorithm. On-line coupled into a meso-scale weather forecast model (MM5), its performance and improvements for aerosol chemical and optical simulations have been evaluated using the observations data of aerosols/gases from the intensive observations and from the CMA Atmosphere Watch network, plus aerosol optical depth (AOD) data from CMA Aerosol Remote Sensing network (CARSNET) and from Moderate Resolution Imaging Spectroradiometer (MODIS). Targeting Beijing and North China region from July 13 to 31, 2008, when a heavy hazy weather system occurred, the model captured the general variations of PM10 with most of the data within a factor of 2 from the observations and a combined correlation coefficient (r) of 0.38 (significance level=0.05). The correlation coefficients are better at rural than at urban sites, and better at daytime than at nighttime. Chemically, the correlation coefficients between the daily-averaged modelled and observed concentrations range from 0.34 for black carbon (BC) to 0.09 for nitrates with sulphate, ammonium and organic carbon (OC) in between. Like the PM10, the values of chemical species are higher for the daytime than those for the nighttime. On average, the sulphate, ammonium, nitrate and OC are underestimated by about 60, 70, 96.0 and 10.8%, respectively. Black carbon is overestimated by about 120%. A new size distribution for the primary particle emissions was constructed for most of the anthropogenic aerosols such as BC, OC, sulphate, nitrate and ammonium from the observed size distribution of atmospheric aerosols in Beijing. This not only improves the correlation between the modelled and observed AOD, but also reduces the overestimation of AOD simulated by the original model size distributions of primary aerosols. The normalised mean error has been reduced to 62% with the CARSNET observations and 76% with MODIS, from the original 111% and 143%, respectively. The factors resulting in the underestimation of aerosol concentrations and other discrepancies in the model are explored, and improvements in enhancing the model performance are proposed from the analysis. It is found that the accuracy in meteorological predictions plays a critical role on the simulation of the occurrence and accumulation of heavy pollution episode, especially the circulation winds and the treatment of Planetary Boundary Layer (PBL).

[1]  David R. Stauffer,et al.  Turbulence in the nocturnal boundary layer with light and variable winds , 2012 .

[2]  Y. Q. Wang,et al.  Atmospheric aerosol compositions in China: Spatial/temporal variability, chemical signature, regional haze distribution and comparisons with global aerosols , 2011 .

[3]  Y. Q. Wang,et al.  Spatial distribution and interannual variation of surface PM 10 concentrations over eighty-six Chinese cities , 2010 .

[4]  H. Che,et al.  CHANGES OF ATMOSPHERIC COMPOSITION AND OPTICAL PROPERTIES OVER BEIJING—2008 Olympic Monitoring Campaign , 2009 .

[5]  P. Goloub,et al.  Instrument calibration and aerosol optical depth validation of the China Aerosol Remote Sensing Network , 2009 .

[6]  Dingli Yue,et al.  Characteristics of aerosol size distributions and new particle formation in the summer in Beijing , 2009 .

[7]  A. Khain Notes on state-of-the-art investigations of aerosol effects on precipitation: a critical review , 2009 .

[8]  W. Cotton,et al.  Aerosol Pollution Impact on Precipitation , 2009 .

[9]  W. Cotton,et al.  Aerosol pollution impact on precipitation : a scientific review , 2009 .

[10]  Xiaoye Zhang,et al.  Carbonaceous aerosol composition over various regions of China during 2006 , 2008 .

[11]  R. Mathur,et al.  Evaluation of real‐time PM2.5 forecasts and process analysis for PM2.5 formation over the eastern United States using the Eta‐CMAQ forecast model during the 2004 ICARTT study , 2008 .

[12]  Evaluation of WRF model improvements with novel boundary-layer observations-Focus on diurnal cycle and stable boundary layer , 2008 .

[13]  S. Parkd,et al.  MICS-Asia II : The model intercomparison study for Asia Phase II methodology and overview of findings , 2008 .

[14]  Teruyuki Nakajima,et al.  Overview of the Atmospheric Brown Cloud East Asian Regional Experiment 2005 and a study of the aerosol direct radiative forcing in east Asia , 2007 .

[15]  H. Che,et al.  Inventory of Black Carbon Emission from China , 2007 .

[16]  E. Vermote,et al.  Second‐generation operational algorithm: Retrieval of aerosol properties over land from inversion of Moderate Resolution Imaging Spectroradiometer spectral reflectance , 2007 .

[17]  Y. Q. Wang,et al.  Development and evaluation of an operational SDS forecasting system for East Asia: CUACE/Dust , 2007 .

[18]  Stefano Schiavon,et al.  Climate Change 2007: The Physical Science Basis. , 2007 .

[19]  G. Grell,et al.  Evolution of ozone, particulates, and aerosol direct radiative forcing in the vicinity of Houston using a fully coupled meteorology‐chemistry‐aerosol model , 2006 .

[20]  V. Ramanathan,et al.  Influence of aerosols on the shortwave cloud radiative forcing from North Pacific oceanic clouds: Results from the Cloud Indirect Forcing Experiment (CIFEX) , 2006 .

[21]  J. Dudhia,et al.  A New Vertical Diffusion Package with an Explicit Treatment of Entrainment Processes , 2006 .

[22]  Piotr K. Smolarkiewicz,et al.  Multidimensional positive definite advection transport algorithm: an overview , 2006 .

[23]  E. Maisonnave,et al.  West African monsoon response to greenhouse gas and sulphate aerosol forcing under two emission scenarios , 2006 .

[24]  C. Jia,et al.  A Study of Evolution and Dynamics of Urban Atmospheric Mixing-Layer Depth Based on Lidar Data and Numerical Simulation , 2006 .

[25]  Shaocai Yu,et al.  New unbiased symmetric metrics for evaluation of air quality models , 2006 .

[26]  W. Collins,et al.  An AeroCom initial assessment – optical properties in aerosol component modules of global models , 2018 .

[27]  J. Burrows,et al.  Increase in tropospheric nitrogen dioxide over China observed from space , 2005, Nature.

[28]  Jenise L. Swall,et al.  An assessment of the ability of three‐dimensional air quality models with current thermodynamic equilibrium models to predict aerosol NO3− , 2005 .

[29]  Zheng Fang-cheng,et al.  Inventory of atmospheric pollutants discharged from biomass burning in China continent , 2005 .

[30]  S. Liu,et al.  Model simulation and analysis of coarse and fine particle distributions during ACE‐Asia , 2004 .

[31]  J. Seinfeld,et al.  Three-dimensional simulations of inorganic aerosol distributions in east Asia during spring 2001 , 2004, Journal of Geophysical Research.

[32]  O. Boucher,et al.  The aerosol-climate model ECHAM5-HAM , 2004 .

[33]  William C. Malm,et al.  Spatial and monthly trends in speciated fine particle concentration in the United States , 2004 .

[34]  Jenise L. Swall,et al.  An assessment of the ability of 3-D air quality models with current thermodynamic equilibrium models to predict aerosol NO 3 - , 2004 .

[35]  I. McKendry,et al.  Modeled size‐segregated wet and dry deposition budgets of soil dust aerosol during ACE‐Asia 2001: Implications for trans‐Pacific transport , 2003 .

[36]  Mian Chin,et al.  A global aerosol model forecast for the ACE-Asia field experiment , 2003 .

[37]  S. Gong,et al.  A parameterization of sea‐salt aerosol source function for sub‐ and super‐micron particles , 2003 .

[38]  Clouds and trace gas distributions during TRACE-P , 2003 .

[39]  David G. Streets,et al.  Large‐scale structure of trace gas and aerosol distributions over the western Pacific Ocean during the Transport and Chemical Evolution Over the Pacific (TRACE‐P) experiment , 2003 .

[40]  Michael Q. Wang,et al.  An inventory of gaseous and primary aerosol emissions in Asia in the year 2000 , 2003 .

[41]  C. Timmreck,et al.  Monthly Averages of Aerosol Properties: A Global Comparison Among Models, Satellite Data, and AERONET Ground Data , 2003 .

[42]  Petr Chylek,et al.  Canadian Aerosol Module: A size‐segregated simulation of atmospheric aerosol processes for climate and air quality models 1. Module development , 2003 .

[43]  A. Berger,et al.  Are Natural Climate Forcings Able to Counteract the Projected Anthropogenic Global Warming? , 2002 .

[44]  Xiao-yan Tang,et al.  [Determination and characteristics of OH radical in urban atmosphere in Beijing]. , 2002, Huan jing ke xue= Huanjing kexue.

[45]  Frances Silverman,et al.  Inhalation of Fine Particulate Air Pollution and Ozone Causes Acute Arterial Vasoconstriction in Healthy Adults , 2002, Circulation.

[46]  V. Ramanathan,et al.  Aerosols, Climate, and the Hydrological Cycle , 2001, Science.

[47]  J. Veefkind,et al.  Simulation of the aerosol optical depth over Europe for August 1997 and a comparison with observations , 2001 .

[48]  I. J. Ackermann,et al.  Modeling the formation of secondary organic aerosol within a comprehensive air quality model system , 2001 .

[49]  L. Gomes,et al.  Modeling mineral aerosol production by wind erosion: Emission intensities and aerosol size distributions in source areas , 2001 .

[50]  Shaocai Yu,et al.  A comparison of signals of regional aerosol‐induced forcing in eastern China and the southeastern United States , 2001 .

[51]  J. Seinfeld,et al.  General circulation model assessment of direct radiative forcing by the sulfate-nitrate-ammonium-water inorganic aerosol system , 2001 .

[52]  Shaocai Yu Role of organic acids formic, acetic, pyruvic and / oxalic in the formation of cloud condensation / nuclei CCN : a review , 2000 .

[53]  A. Nenes,et al.  Continued development and testing of a new thermodynamic aerosol module for urban and regional air quality models , 1999 .

[54]  J. Seinfeld,et al.  Simulation of Aerosol Dynamics: A Comparative Review of Algorithms Used in Air Quality Models , 1999 .

[55]  R. Arimoto,et al.  Concentration, size-distribution and deposition of mineral aerosol over Chinese desert regions , 1998 .

[56]  A. Nenes,et al.  Marginal direct climate forcing by atmospheric aerosols , 1998 .

[57]  E. Vermote,et al.  Operational remote sensing of tropospheric aerosol over land from EOS moderate resolution imaging spectroradiometer , 1997 .

[58]  M. Jacobson Development and application of a new air pollution modeling system-part I: Gas-phase simulations , 1997 .

[59]  R. Hitzenberger,et al.  Modal character of atmospheric black carbon size distributions , 1996 .

[60]  B. Marticorena,et al.  Modeling the atmospheric dust cycle: 1. Design of a soil-derived dust emission scheme , 1995 .

[61]  R. Charlson,et al.  Aerosol forcing of climate : report of the Dahlem Workshop on Aerosol Forcing of Climate, Berlin 1994, April 24-29 , 1995 .

[62]  D. L. Roberts,et al.  A climate model study of indirect radiative forcing by anthropogenic sulphate aerosols , 1994, Nature.

[63]  S. Twomey,et al.  Aerosols, clouds and radiation , 1991 .

[64]  W. Stockwell,et al.  The second generation regional acid deposition model chemical mechanism for regional air quality modeling , 1990 .

[65]  M. C. Dodge,et al.  A photochemical kinetics mechanism for urban and regional scale computer modeling , 1989 .

[66]  E. Wolf,et al.  The Study of Evolution , 1970 .

[67]  G. P. Cressman AN OPERATIONAL OBJECTIVE ANALYSIS SYSTEM , 1959 .