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NASA Technical Reports Server (NTRS) 20140005403: New Approach to Monitor Transboundary Particulate Pollution over Northeast Asia PDF

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Atmos.Chem.Phys.,14,659–674,2014 Atmospheric O p www.atmos-chem-phys.net/14/659/2014/ e Chemistry n doi:10.5194/acp-14-659-2014 A c and Physics c ©Author(s)2014.CCAttribution3.0License. e s s New approach to monitor transboundary particulate pollution over Northeast Asia M.E.Park1,C.H.Song1,R.S.Park1,J.Lee2,3,4,J.Kim2,S.Lee1,J.-H.Woo5,G.R.Carmichael6,T.F.Eck4,7, B.N.Holben4,S.-S.Lee8,C.K.Song9,andY.D.Hong9 1SchoolofEnvironmentalScienceandEngineering,GwangjuInstituteofScienceandTechnology(GIST),Gwangju, 500-712,Korea 2DepartmentofAtmosphericSciences,YonseiUniversity,Seoul,120-749,Korea 3EarthSystemScienceInterdisciplinaryCenter,UniversityofMaryland,CollegePark,Maryland,USA 4LaboratoryforTerrestrialPhysics,GoddardSpaceFlightCenter,NationalAeronauticsandSpaceAdministration(NASA), Greenbelt,Maryland,USA 5DepartmentofAdvancedTechnologyFusion,KonkukUniversity,Seoul,143-701,Korea 6DepartmentofChemicalandBiochemicalEngineering,UniversityofIowa,IowaCity,Iowa,USA 7UniversitiesSpaceResearchAssociation,Columbia,Maryland,USA 8NationalInstituteofMeteorologicalResearch,Seoul,156-720,Korea 9AirQualityResearchDepartment,NationalInstituteofEnvironmentalResearch(NIER),Incheon,404-170,Korea Correspondenceto:C.H.Song([email protected]) Received:29March2013–PublishedinAtmos.Chem.Phys.Discuss.:14June2013 Revised:29November2013–Accepted:3December2013–Published:22January2014 Abstract. A new approach to more accurately monitor and pared to background average AOD (aerosol optical depth) evaluate transboundary particulate matter (PM) pollution is at the four AERONET sites in Korea, and average AOD in- introduced based on aerosol optical products from Korea’s creases of 121% were found when averaged over the entire Geostationary Ocean Color Imager (GOCI). The area stud- Korean peninsula. This paper demonstrates that the use of ied is Northeast Asia (including eastern parts of China, the multi-spectral AOD retrievals from geostationary satellites Korean peninsula and Japan), where GOCI has been mon- canimproveestimatesoftransboundaryPMpollution.Such itoring since June 2010. The hourly multi-spectral aerosol data will become more widely available later this decade optical data that were retrieved from GOCI sensor onboard when new sensors such as the GEMS (Geostationary Envi- geostationary satellite COMS (Communication, Ocean, and ronment Monitoring Spectrometer) and GOCI-2 are sched- Meteorology Satellite) through the Yonsei aerosol retrieval uledtobelaunched. algorithm were first presented and used in this study. The GOCI-retrievedaerosolopticaldataareintegratedwithesti- mated aerosol distributions from US EPA Models-3/CMAQ (Community Multi-scale Air Quality) v4.5.1 model simu- 1 Introduction lations via data assimilation technique, thereby making the aerosoldataspatiallycontinuousandavailableevenforcloud Transboundary air pollution is an important issue in Asia contaminationcells.Theassimilatedaerosolopticaldataare (Arndt et al., 1998; Holloway et al., 2002; Yamaji et al., utilized to provide quantitative estimates of transboundary 2012). In particular, the long-range transport (LRT) of air PMpollutionfromChinatotheKoreanpeninsulaandJapan. pollutants from China (source) to the Korean peninsula and Fortheperiodof1Aprilto31May,2011thisanalysisyields Japan (receptors) due to persistent westerlies over North- estimates that AOD as a proxy for PM2.5 or PM10 during east Asia has been a central issue in this region (Arndt et long-range transport events increased by 117–265% com- al.,1998;SongandCarmichael,2001;Yamajietal.,2012). Transboundary air pollution is a serious issue not only in PublishedbyCopernicusPublicationsonbehalfoftheEuropeanGeosciencesUnion. 660 M.E.Parketal.:Transboundaryparticulatepollution Asia,butalsoinEuropeandNorthAmerica,causinganum- theUSAGOESseries(GOES8,13),theJapaneseGMSand ber of different international problems such as acid precipi- MTSAT, and European SEVIRI have been meteorological tation, rising levels of hemispheric ground-level ozone, and sensors with only one to two visible channels. The history regional visibility impairment (Levy II and Moxim, 1987; ofGEOsatellitesensorsfortheretrievaloftheaerosolopti- Brankov et al., 2003; Holloway et al., 2003; Tulet et al., calpropertiesissummarizedinTable1. 2003;Parketal.,2004;Wangetal.,2009).Tomanagetrans- This situation is changing as new geostationary satel- boundaryairpollutionbetweencountries,theConventionon lite based sensors are becoming available and will be ex- Long-Range Transboundary Air Pollution (CLRTAP) under panded by upcoming planned missions. The first hourly theUNECE(UnitedNationsEconomicCommissionforEu- multi-spectral aerosol data observed from a geostationary rope) was launched to lessen air pollution through the LRT satellite sensor, GOCI (Geostationary Ocean Color Imager) in1979(http://www.unece.org/env/lrtap/lrtap_h1.html).The is used in this paper to demonstrate how this new informa- EMEP(EuropeanMonitoringandEvaluationProgramme)is tion can be used to improve our estimates of LRT of pol- ascientificeffortestablishedtosupporttheCLRTAP. lutants. Specifically, the level 1 radiance data from GOCI, Quantitative evaluation of transboundary air pollution re- onboard COMS (Communication, Ocean, and Meteorology mains a difficult task and currently cannot be done based Satellite), is converted into level 2 AOD products via the on observations alone due to a lack of explicit source sig- “Yonsei aerosol retrieval algorithm” (the details of the al- naturesandlackofanappropriateobservationsystem(Mal- gorithm will be discussed in the Methods section) (Lee et colm et al., 2000; Brankov et al., 2003; Tulet et al., 2003; al.,2010).COMS/GOCIwaslaunchedinJune2010,andthe Park et al., 2004; Schaub et al., 2005; Wang et al., 2009). COMS/GOCI data center began to release radiance data in Most current evaluations of transboundary transport of pol- April2011,afteraninitialoperationtest(IOT)period.This lutantsarebasedonchemistry-transportmodel(CTM)sim- satellite sensor was designed for monitoring ocean colors ulations(LevyIIandMoxim,1987;Arndtetal.,1998;Hol- around the Korean peninsula, but it can also provide AOD lowayetal.,2002;Wangetal.,2009;Yamajietal.,2012).By dataforastrategicallyimportantregion,i.e.,NortheastAsia. controllingtheemissionsfromasourcecountry(e.g.,China) The domain covered by the GOCI sensor shown in Fig. 1 intheCTMsimulations,transboundaryairpollutionfromthe is 2500km×2500km and includes eastern parts of China, sourcecountrytoreceptorregionshasbeenevaluated.How- theKoreanpeninsula,andJapan.TheGOCI-retrievedAOD ever, these model-based evaluations have significant limita- products were integrated with CMAQ-simulated AOD data tionsbecauseofthelargeuncertaintiesintheemissionrates toproducethemoreaccurateaerosoldatasetusedtoinvesti- of the air pollutants from the source country (or region), gatetheimpactsoftransboundaryPMpollutionbetweenthe the highly nonlinear nature of atmospheric chemistry, and sourceandreceptorcountriesinNortheastAsia. uncertainties related to the CTM and meteorological mod- els (MM). For example, both atmospheric secondary parti- 2 Methods cle formation and primary particle (e.g., mineral dust) gen- eration/transportaredifficulttocorrectlysimulate(Songand The procedure to produce GOCI-constrained AOD product Carmichael,2001;Songetal.,2005;Volkameretal.,2006; combines the GOCI level 2 product with AOD predictions Robinsonetal.,2007).Theseuncertaintiesareamainreason fromtheUSEPAModel-3/CMAQ(CommunityMulti-scale for disagreement in source and receptor estimates made by Air Quality) v4.5.1 model simulations. The CMAQ model differentcountries,whichhasledtodistrustoftheoutcomes simulations were performed over East Asia, with emission ofmodel-basedassessments. datapreparedappropriatelyforthemodeldomainandmete- Current efforts to reduce the uncertainty in estimates of orological fields produced from the PSU/NCAR MM5 (the long-rangetransportofpollutantsbyintegratingmodelsand fifth generation meteorological model) simulations. The fi- observationsthroughdataassimilationarelimitedbyourcur- nal AOD product is spatially continuous and available even rent observational systems. Surface-based observations are for locations where GOCI retrievals are not available (e.g., toosparsetoconstrainthesystem,whilecurrentsatellitesare cloud-contaminatedpoints,sun-glintareas,desert,andsnow- unabletoretrieveaerosolconcentrations.Instead,satellitere- covered land). The use of GOCI-retrievals overcomes the trievalsofAODareusedtohelpconstrainmodeledAODand “temporal limitation” typical in analyses with LEO (low themodeledrelationshipbetweenAODandsurface-levelPM Earthorbit)aerosoldataandtheassimilationovercomesthe (particulatematter)canthenbeusedtoestimatesurface-level “spatial limitation” that has been typical in analyses based PMconcentrations(WangandChristopher,2003;Liuetal., onlyonsatellitedata.TheassimilatedAODdatasetusingthe 2005;vanDonkelaaretal.,2006;Schaapetal.,2009;Tsaiet GOCIdataisutilizedtomonitorandevaluatetransboundary al.,2011).Thisapproachiscurrentlylimitedbythefactthat particulate pollution from China to the Korean peninsula in AOD from polar-orbiting satellites produce retrievals only thisstudy. once per day (Kaufman et al., 1997; Diner et al., 2001) and currentgeostationarysatelliteslack“multi-spectral”aerosol data (Knapp et al., 2002; Wang et al., 2003). For example, Atmos.Chem.Phys.,14,659–674,2014 www.atmos-chem-phys.net/14/659/2014/ M.E.Parketal.:Transboundaryparticulatepollution 661 Table1.Briefdescriptionsofaerosolopticalpropertyretrievalsfromsomegeostationarysatellites. Satellite& GMS51 MTSAT-1R2 MSG3 GOES4 COMS5 GOES-R GEO-KOMPSAT6 Sensor VISSR7 JAMI8 SEVIRI9 GOES-8 GOCI10 ABI11 GEMS12&ABI& GOCI-2 Sensortype MET13sensor METsensor METsensor METsensor Oceancolorimager METsensor Environ.&ocean colorimager Temporalresolution 1h 30min 15min 15min 1h TBD17 1h(GEMS) Spatialresolution a1.25km/b5km 1.25km/5km 1km/3km 1km/4km 0.5km/0.5km 0.5km/2km 0.25km/1km Numberofbands 1VIS14/3IR16 1VIS/4IR 2VIS/2NIR15/ 1VIS/4IR 6VIS/2NIR 2VIS/4NIR/ 13VIS/NIR 8IR 10IR Coveringregion EastAsia EastAsia Central Eastern Northeast US East,Southeast &westernPacificOcean &westernPacificOcean Europe US Asia &CentralAsia Launchyear Mar1995 Feb2005 Aug2002 Apr1994 Jun2010 Scheduledtobe Scheduledtobe launchedin2015 launchedin2018 References Masudaetal.(2002); Kimetal.(2008) Poppetal.(2007) Christopheretal.(2002); Leeetal.(2010); Laszloetal.(2008) Wangetal.(2003) Knappetal.(2002,2005) thisstudy 1GMS:GeostationaryMeteorologicalSatellite,2MTSAT-1R:Multi-functionalTransportSatellite,3MSG:MeteosatSecondGeneration,4GOES:GeostationaryOperationalEnvironmentalSatellite,5COMS:Communication,Ocean,andMeteorological Satellite,6GEO-KOMPSAT:GeostationaryEarthOrbitKOreaMulti-PurposeSATellite,7VISSR:VisibleandInfraRedSpinScanRadiometer,8JAMI:JapaneseAdvancedMeteorologicalImager,9SEVIRI:SpinningEnhancedVisibleandInfraRedImager, 10GOCI:GeostationaryOceanColorImager,11ABI:AdvancedBaselineImager,12GEMS:GeostationaryEnvironmentMonitoringSpectrometer,13MET:Meteorological,14VIS:VISible,15NIR:NearInfraRed,16IR:InfraRed,17TBD:ToBe Determined,aResolutionforthevisiblechannels,bResolutionfortheinfraredchannels. 2.1 Meteorologyandchemistry-transportmodel simulations N CMAQ domain 0 5 ThePSU/NCARMM5andUSEPAModel-3/CMAQmodel GOCI domain v4.5.1 were respectively used as the meteorological model N (A) (MM) and chemistry-transport model (CTM) in this study 40 (cid:36)(cid:67)(cid:71)(cid:80)(cid:73)(cid:80)(cid:91)(cid:71)(cid:81)(cid:80)(cid:73) (B) (cid:59)(cid:81)(cid:80)(cid:85)(cid:71)(cid:75)(cid:65)(cid:55)(cid:80)(cid:75)(cid:88) (cid:59)(cid:71)(cid:78)(cid:78)(cid:81)(cid:89) (C) (Byun and Schere, 2006; Park et al., 2011). The accuracy (cid:41)(cid:53)(cid:89)(cid:71)(cid:67)(cid:67)(cid:80)(cid:73)(cid:76)(cid:87)(cid:65)(cid:41)(cid:43)(cid:53)(cid:54) (cid:49)(cid:85)(cid:67)(cid:77)(cid:67) (cid:41)(cid:81)(cid:85)(cid:67)(cid:80)(cid:65)(cid:53)(cid:48)(cid:55) of the MM5 simulations was enhanced by nudging with 30N (cid:37)(cid:74)(cid:39)(cid:75)(cid:80)(cid:67)(cid:67)(cid:85)(cid:86)(cid:53)(cid:71)(cid:67) the observed meteorological data (Grell et al., 1995). Ini- tial conditions (ICs) and boundary conditions (BCs) for the MM5 simulations were updated continuously with the Na- 0N 2 tionalCentersforEnvironmentalPrediction(NCEP)reanal- ysis data. The latest remotely sensed surface wind data re- 90E 100E 110E 120E 130E 140E 150E trievedfromtheAdvancedSCATterometer(ASCAT),which was launched on 19 October 2006 onboard the Meteoro- N 2 logical Operational satellite A (MetOp-A) was used for 4 (A) the four-dimensional data assimilation (FDDA), since dur- (cid:36)(cid:67)(cid:71)(cid:80)(cid:73)(cid:80)(cid:91)(cid:71)(cid:81)(cid:80)(cid:73) N ing regional-scale, long-range transport events the signif- 38 (B) (cid:59)(cid:71)(cid:78)(cid:78)(cid:81)(cid:89) (cid:59)(cid:81)(cid:80)(cid:85)(cid:71)(cid:75)(cid:65)(cid:55)(cid:80)(cid:75)(cid:88) icant fractions of air pollutants are frequently transported (cid:53)(cid:71)(cid:67) (C) throughthemarineboundarylayer(MBL)betweencountries N (cid:41)(cid:89)(cid:67)(cid:80)(cid:73)(cid:76)(cid:87)(cid:65)(cid:41)(cid:43)(cid:53)(cid:54) 4 inNortheastAsia(e.g.,throughtheMBLovertheYellowSea 3 (cid:41)(cid:81)(cid:85)(cid:67)(cid:80)(cid:65)(cid:53)(cid:48)(cid:55) betweenChinaandKoreaandthroughtheMBLovertheEast 124E 128E 132E ChinaSeabetweenChinaandJapan;regardingthelocations of the Yellow Sea and the East China Sea, refer to Fig. 1) Fig. 1. Domains of CMAQ model simulations (in blue) and COMS/GOCIsensor(inred).AlsoshownarefiveAERONETsites (Daumetal.,1996;Rajeevetal.,2000;Songetal.,2007). inthereceptorareas(KoreaandJapan).Forthesakeofanalytical The schemes chosen for CMAQ model simulations were convenience,threesubregions(A),(B),and(C)intheKoreanpenin- the same as those used in previous research (Park et al., sulaaredefined;theserepresentthenorthern,central,andsouthern 2011). The SAPRC-99 chemical mechanism and AERO4 partsoftheKoreanpeninsula,respectively. aerosol module were selected for simulating gas-phase chemistryandatmosphericaerosolthermodynamic/dynamic processes,respectively.MoredetailsoftheMM5andCMAQ model simulations were described in a previous publication tionalCenterforAtmosphericResearch)FINN(FireInven- (Parketal.,2011). tory from NCAR) biomass-burning (BB) emissions (Wied- TheCMAQmodelsimulationswerecarriedoutusingthe inmyeretal.,2011).TheeffortsaresummarizedinTable2. best available emission inventories over East Asia that have Fortheconsiderationofanthropogenicpollutantsemissions, been made more sophisticated with, for example, the appli- suchasNO ,SO ,CO,blackcarbon(BC),NMVOCs,etc., x 2 cations of monthly variations of anthropogenic emissions, Intercontinental Chemical Transport Experiment-Phase B the uses of an operational dust forecast model at the KMA (INTEX-B), Regional Emission inventory in Asia (REAS), (KoreaMeteorologicalAdministration)andtheNCAR(Na- andCleanAirPolicySupportSystem(CAPSS)wereapplied www.atmos-chem-phys.net/14/659/2014/ Atmos.Chem.Phys.,14,659–674,2014 662 M.E.Parketal.:Transboundaryparticulatepollution as the best suitable emission data over China, Japan, and 2.2 Remote-sensingdata theKoreanpeninsula,respectively.Theseemissioninvento- ries originally adjusted to the year 2006 were updated for 2.2.1 COMS/GOCIdata the year 2011 modeling period, using the projection fac- torsbasedontheGreenhousegasandAirpollutionINterac- SensorsonboardLEOsatellites,suchasMODIS(Moderate tionsandSynergies(GAINS)modelingemissionsscenarios Resolution Imaging Spectroradiometer) and MISR (Multi- (http://gains.iiasa.ac.at/index.php/gains-asia). In the mean- angleImagingSpectroradiometer),haveordinarilybeenuti- while,inordertoconsiderisopreneandmonoterpeneemis- lized to obtain information on aerosol optical properties sionsoverthemodelingdomain,theisopreneemissionsfrom (AOPs), but their monitoring has taken place at most once Model of Emissions of Gases and Aerosols from Nature per day. To more accurately monitor the transboundary (MEGAN) and MOdel for Hydrocarbon emissions by the LRT events of air pollutants, hourly (or highly temporally CANopy(MOHYCAN)wereutilizedfortheCMAQmodel- resolved) monitoring data from geostationary Earth orbit inginputdata(Mülleretal.,2008).Monoterpeneemissions (GEO) sensors are needed instead of the temporally lim- were also estimated from the isoprene emissions, using the ited LEO measured data. As mentioned previously and also ratiosofmonoterpenetoisoprenefromGlobalEmissionsIn- presented in Table 1, MSG, GOES, and MTSAT-1R sen- ventoryActivity(GEIA). sors have been partly monitoring the AOPs over Europe, In particular, this modeling period (a spring season in US, and Japan, respectively (Knapp et al., 2005; Popp et Northeast Asia)could not be explained without considering al., 2007; Kim et al., 2008), but these meteorological sen- the effects of BB and mineral dust emissions. FINNv1 is a sorsareequippedwithonlyonevisiblechannel,whichpos- BBemissioninventoryannuallyprovidedfromtheyear2002 sibly makes the quality of the AOPs from these meteoro- by NCAR (http://bai.acd.ucar.edu/Data/fire/). This FINNv1 logical sensors less accurate. In contrast, GOCI sensor on- has produced the BB emission data with a high horizontal board geostationary COMS has six visible bands at 412, resolutionof∼1km×1kmovertheentireglobe,beingap- 443, 490, 555, 660, 680 nm, which can make advances by pliedforvariableregionsfromlocaltoglobalscales(Wied- more accurately calculating the AOPs, compared to other inmyeretal.,2011).Inthisstudy,theFINNv1wasusedfor meteorological GEO satellite sensors. In addition, atmo- the BB emissions. The CMAQ v4.5.1 model does not in- spheric compensations, such as cloud-screening make the clude any dust modeling modules related to occurrence and numerical accuracy of the AOPs more improved, because transportofmineraldustevents.However,withouttakingthe the COMS/GOCI has 2 more bands at 745nm and 865nm influence of mineral dust events into account, accurate esti- (i.e.,nearIR).TheGOCIsensorcoversNortheastChina,the mationoftheaerosolseffectsobservedbylong-rangetrans- Korean peninsula, and Japan, and the products can be gen- portsintheKoreanpeninsulaandJapanwouldnotbepossi- erated with 500m×500m spatial resolution. GOCI level 1 ble. Therefore, the outbreak and transport of Asian mineral dataduringdaytimecanbeobtainedeighttimesfrom09:00 dustwereconsideredbyAsianDustAerosolModel(ADAM) to16:00LST(localstandardtime)(refertohttp://kosc.kordi. simulations. The ADAM is currently operational model for re.kr/oceansatellite/coms-goci/introduction.kosc). forecasting Asian mineral dust events at the KMA and the ThehourlyGOCIlevel1dataisreleasedsomewhatslowly details of the ADAM simulations were reported previously after the IOT and data calibration procedures. The GOCI bye.g.,ParkandLee(2004),Kimetal.(2011),andParket level 1 radiance is then converted into level 2 AOD data al.(2011). using a multi-spectral algorithm being developed by Jhoon ThedomainoftheCMAQmodelsimulationisalsoshown Kim and coworkers at Yonsei University, Korea (Lee et al., in Fig. 1. The CMAQ domain (blue color) covered the re- 2010). The level 2 AOD data retrieved with a pixel size of gionofapproximately95–145◦E,20–50◦N,whichincludes 6km×6km was used in this study. The retrieval algorithm COMS/GOCI domain (red color) composed of Northeast was originally based on the NASA MODIS (i.e., LEO) al- China, the Korean peninsula, and Japan. In this study, the gorithm, but it has evolved to date to include the aerosol CMAQ domain was chosen to be larger than the GOCI modelsoptimizedforEastAsiaandtoconsiderthegeometry domain, since the air quality inside the GOCI domain is fromGEOsatelliteinstrumentssuchasGOCI,GOCI-2,and stronglyinfluencedbytheinfluxesfromtheouterareaswith GEMS(GeostationaryEnvironmentMonitoringSpectrome- persistent westerlies in East Asia. The horizontal grid spac- ter) (both the GOCI-2 and GEMS sensors are scheduled to ing of the CMAQ modeling was 30km×30km and the belaunchedin2018).TheYonseiaerosolretrievalalgorithm vertical domain was distributed in 14 layers following σ- includesthecapabilitytoclassifyaerosoltypesbasedonab- coordinatefrom1000hPato70hPa.TheMM5-CMAQsim- sorptiontestsandsizeinformation(Kimetal.,2007;Leeet ulation period started at 00:00UTC, 1 April to 23:00UTC, al.,2010).TheevaluationofthecurrentAODdatafromthe 31 May 2011 (with a week-long CMAQ spin-up period), algorithm shows that the slope of the linear regression line since the first batch of the level1 radiance data from the is close to 1.03 over ocean, but 1.15 over land when com- COMS/GOCIdatacenterwasreleasedforthisperiod. pared to values from AERONET. Although the detailed ex- planation and validation procedures of this Yonsei aerosol Atmos.Chem.Phys.,14,659–674,2014 www.atmos-chem-phys.net/14/659/2014/ M.E.Parketal.:Transboundaryparticulatepollution 663 Table2.EmissioninventoriesusedintheCMAQmodelsimulations. Region Emissioninventory Species ChinaandNorthKorea INTEX-B1 SO2,NOx,NMVOCs,CO,CO2,BC,OC EDGAR2 NH3 SouthKorea CAPSS3 SO2,NOx,NMVOCs,CO,NH3 INTEX-B CO2,BC,OC,ChemicalsplitfactorsofNMVOCs Japan REAS4 SO2,NOx,NMVOCs,CO,CO2,NH3,BC,OC Entiredomain GAINS5emissionscenarios aInterannualvariationsofCO,NOx,VOC,SO2,NH3,CO2,CH4,PM2.5 FINN6fireemissions CO,NO,NO2,SO2,NH3,NMVOCs,BC,OC,PM2.5,PM10 MEGAN7+MOHYCAN8 Isoprene GEIA9 bRatiosofmonoterpenetoisoprene 1INTEX-B:IntercontinentalChemicalTransportExperiment-PhaseB,2EDGAR:EmissionDatabaseforGlobalAtmosphericResearch,3CAPSS:CleanAirPolicySupport System,4REAS:RegionalEmissioninventoryinASia,5GAINS:GreenhousegasandAirpollutionINteractionsandSynergies,6FINN:FireInventoryfromNCAR, 7MEGAN:ModelofEmissionsofGasesandAerosolsfromNature,8MOHYCAN:MOdelforHydrocarbonemissionsbytheCANopy,9GEIA:GlobalEmissionsInventory Activity,aEmissionincrease(ordecrease)ratesfrom2006to2011fortheairpollutantswereobtainedfromtheGAINSemissionscenarios,bMonoterpeneemissionsarenot includedinMEGAN+MOHYCANemissions.Therefore,theratiosofmonoterpenetoisopreneinthebiogenicemissionswereobtainedfromtheGEIAemissioninventory. retrievalalgorithmweregiveninpreviouspublications(Lee et al., 2010, 2012), a brief introduction on the algorithm is madehere.TheretrievalsoftheAOPswereperformedwith (a) MODIS-retrieved AOD (b) GOCI-retrieved AOD topofatmospherespectralreflectances.ToobtaintheAOPs 120E 130E 140E 120E 130E 140E over the regions including clouds, clouds are screened by N N N spatialvariabilityandthresholdtestsateachpixel.Evenso, 00 45 45 45 : there are limitations to the complete removal of clouds and 0 1 N N N theperfectretrievalofsurfacereflectanceduetothelackof 0 35 35 35 1 IRbandsonGOCI.Therefore,theYonseiaerosolretrievalal- 4/ 0 N N N gorithmeliminatescloudsutilizingameteorologicalimager 25 25 25 (MI) that has 4 IR channels. The MI sensor is also onboard N N N 0 5 5 5 COMS with GOCI. In addition, the Yonsei aerosol retrieval 0 4 4 4 : 3 algorithm is composed of two different retrieval logics that 1 N N N are applied to “continent” including near-coastal turbid wa- 10 35 35 35 terareasand“ocean”,respectively. 4/ 0 N N N Figure 2 presents one example: a comparison of the 25 25 25 Terra/MODIS-retrieved and Aqua/MODIS-retrieved AODs N N N withGOCI-retrievedAODsatapproximately10:00LSTand 00 45 45 45 : 0 13:00LSTon10Apriland12April,respectively.Asshown 1 N N N in Fig. 2, there are agreements in the spatial AOD distri- 12 35 35 35 butions from the two MODIS and GOCI sensors. As dis- 04/ N N N 5 5 5 cussedpreviously,atmosttwosnapshotsofinformationper 2 2 2 day from the LEO sensors (i.e., MODIS) can be obtained, N N N 0 5 5 5 whereas eight snapshots per day from the GEO sensor (i.e., 0 4 4 4 : 3 GOCI) are available. This is an obvious “temporal” advan- 1 N N N tagethatcanbeachievedfromtheGEOsensor.Furthermore, 12 35 35 35 4/ as shown in Fig. 2, the AOD data from the GOCI sensor 0 N N N 5 5 5 showsabetterspatialcoverage,comparedtothosefromthe 2 2 2 120E 130E 140E 120E 130E 140E MODIS(seewhitebandsalongthenorth–southswathinthe MODIS data). This lack of the MODIS data was caused by 0.0 0.3 0.6 0.9 1.2 1.5 sun-glintovertheoceanareas(detailsaboutthesun-glintef- Fig. 2. Snapshots of (a) Terra and Aqua/MODIS-retrieved AODs fectsarediscussedfurtherinAppendixA).Bycontrast,such and (b) GOCI-retrieved AOD over Northeast Asia at 10:00LST lack of the data is not found in the GOCI data. This is an- (Terra/MODIS) and 13:00 LST (Aqua/MODIS) on 10 April and other“spatial”advantagethatcanbeachievedwiththeGEO 12April. sensor. www.atmos-chem-phys.net/14/659/2014/ Atmos.Chem.Phys.,14,659–674,2014 664 M.E.Parketal.:Transboundaryparticulatepollution 2.2.2 AERONET particulate species i at the size bin or particle mode j, re- spectively. The terms related to the MEEs (βij) and the hy- Manystudieshaveusedtheground-basedNASAAERONET groscopicity(fij(RH))havebeendefineddifferentlyinsev- datatoverifymodelingresultsandsatellitemonitoringdata eralstudies,e.g.,d’Almeidaetal.(1991),Malmetal.(1994), (e.g., Chin et al., 2002, 2004; Yumimoto and Takemura, Chin et al. (2002), Malm and Hand (2007), and Park et 2011). The AERONET data measured by sun photometers al.(2011).Accordingtothepreviousinvestigations,theway were utilized in this study to investigate the accuracy of tocomputetheextinctioncoefficients(σ )hasbeenmainly ext CMAQmodelsimulationsandGOCIAOPdata. classifiedintotwocategories.Thefirstmethodistouseem- Inthismanuscript,thedataobtainedfromfiveAERONET pirical equations (e.g., Malm et al., 1994; Malm and Hand, observation sites (i.e., Baengnyeong, Yonsei Univer- 2007;Songetal.,2008;Parketal.,2011).Theothermethod sity (Yonsei_Univ), GIST (Gwangju_GIST), Gosan istousetheequationsobtainedbasedontheMietheory(e.g., (Gosan_SNU), and Osaka) in the Korean peninsula and d’Almeida et al., 1991; Chin et al., 2002). In this study, the Japanwereselectedinordertoanalyzelong-rangetransport methodsfromChinetal.(2002)andParketal.(2011)were effectsoverNortheastAsia.TheAERONETAODlevel2.0 mainlyutilizedandcompared. data used for comparison was obtained from the official Based on the particulate composition and meteorolog- NASA web site at http://aeronet.gsfc.nasa.gov. The only ical parameters obtained from the MM5-CMAQ model exception was the AERONET AOD data for the Yonsei simulations, the AOD was calculated at a wavelength of University (Seoul) site, which were not calibrated. Before 550nm (AOD ), using the conversion algorithms of Chin 550 use,theywereupgradedbyeliminatingsomesporadiccloud etal.(2002),Parketal.(2011),andothers(d’Almeidaetal., contamination of the initial high AOD data (AOD>1.0) 1991;Malmetal.,1994;Hessetal.,1998;MalmandHand, using the meteorological data from the automatic weather 2007): stations (AWS) colocated with Cimel sun photometers. (cid:5) z The uncertainty and possible anomalies in the Cimel sun AOD = σ (550nm)dz, (4) 550 ext photometerAODdataattheYonseiUniversitysitewerealso 0 checked by the Laboratory for Terrestrial Physics at NASA where z represents the vertical height. For example, the Goddard Space Flight Center. AOD uncertainties of 0.01 to CMAQ-simulated AOD products calculated from Park et 0.04wereestimated,mainlyduetocalibration. al. (2011) usually showed underestimations when com- pared to the AERONET AOD data. However, when Chin 2.3 AODcalculationsfromCMAQmodelsimulations et al.’s (2002) conversion algorithm was applied, the AOD values were usually larger than those calculated by Park et Concentrations of nitrate, sulfate, ammonium, organic al.’s (2011) method. These results will be discussed further aerosols (OAs), BC, sea-salt aerosols, and mineral dust are inalatersection. provided as results of the CMAQ model simulations. This aerosolcompositioncanbeconvertedintotheAOPsinclud- 2.4 Dataassimilation ing AOD by considering the mass extinction efficiencies (MEEs) depending on the scattering and absorbing charac- In several previous studies, optimal interpolation (OI) tech- teristicsforeachaerosolcompositionandthehygroscopicity. niquewithaKalmangainmatrixhasbeenemployedtoim- First, the absorption, scattering, and extinction coefficients provethepredictionsofAODandaerosolmassdistributions (σabs, σscat, and σext) were calculated by the following for- with the combination of the modeling results and monitor- mulas: ing data (Collins et al., 2001; Yu et al., 2003; Adhikary et al., 2008; Chung et al., 2010; Park et al., 2011). For exam- σ (λ)=σ (λ)+σ (λ), (1) ext abs scat ple, Adhikary et al. (2008) showed some enhancements in the estimations of the AOD values over Asia by combin- ing the STEM-modeled and MODIS-retrieved data through (cid:2) (cid:3) (cid:4) (cid:4) σabs λ:Mm−1 = ni mj {(1−ωij(λ))·βij(λ)·fij(RH)·[C]ij}, (2) theOItechnique.TheaccuracyoftheAODvalueswasalso greatlyimprovedaftertheapplicationoftheOImethodusing CMAQ-simulated and MODIS-retrieved AOD data (AOD m σscat(cid:2)λ:Mm−1(cid:3)=(cid:4)ni(cid:4)mj {ωij(λ)·βij(λ)·fij(RH)·[C]ij}, (3) AanOdDA(cid:4)O=DoAiOnDEq.+5)K(P[AarOkDeta−l.,H2(0A1O1)D. )], (5) where i and j represent the particulate species i at the size m m o m bin or particle mode j; fij(RH) the hygroscopic enhance- ment factor as a function of relative humidity (RH); [C]ij K=BHT(HBHT+O)−1, (6) theconcentrationsofparticulatespeciessuchas(NH ) SO , 4 2 4 NH NO ,BC,OAs,mineraldust,andsea-saltaerosols;and whereHdenotesalinearoperatorforinterpolationfromthe 4 3 ωij(λ) and βij(λ) the single scattering albedo and MEE of modelinggridtothesatelliteretrievalgrid.BandOrepresent Atmos.Chem.Phys.,14,659–674,2014 www.atmos-chem-phys.net/14/659/2014/ M.E.Parketal.:Transboundaryparticulatepollution 665 theerrorcovariancesofthemodelingandsatellite(observa- (a) CMAQ AOD (b) GOCI AOD (c) Assimilated AOD tion)fields,respectively. 120E 130E 140E 120E 130E 140E 120E 130E 140E N N N N In this study, the OI technique was again utilized for the 00 45 45 45 45 assimilationoftheAODdatafromtheGOCIsensorintothe 09: N N N N CobMtaAinQedmboydethl.eTchoevaKriaalnmceanofgaminodmelaetdrixan(dKoibnseErvqe.d6)fiewldass 04/10 25N35 25N35 25N35 25N35 (B and O in Eq. 6) which is a function of free parameters. 00 45N 45N 45N 45N Terhael pyreeavriloyufisxsetdudfireese(pCaorallminesteertsawl.,er2e0m01a;inYluy uetseadl.,in20s0ev3-; 4/10 11: 35N 35N 35N 35N 0 N N N N Adhikary et al., 2008; Chung et al., 2010), whereas Park et 25 25 25 25 al. (2011) proposed applying seasonal variations of free pa- 00 45N 45N 45N 45N rameters.Thebestfreeparametersforfourseasonssuggested 3: 1 N N N N in Park et al. (2011) were used here. Detailed explanations 10 35 35 35 35 4/ of the OI technique including the selection of the free pa- 0 25N 25N 25N 25N rameters were made in Park et al. (2011). The assimilated N N N N 00 45 45 45 45 AODdataproducedbycombiningtheCMAQ-simulatedand 5: 1 N N N N theGOCI-retrievedAODswereusedtoinvestigatethelong- 10 35 35 35 35 4/ rangePMtransporteventsinthisstudy. 0 N N N N 25 25 25 25 120E 130E 140E 120E 130E 140E 120E 130E 140E 2.5 Long-rangetransportofparticulatematter 0.0 0.3 0.6 0.9 1.2 1.5 Fig.3.Spatialandtemporaldistributionsof(a)CMAQ-simulated TransboundarytransportsoftheAODplumesfromtheChina AOD (calculated via Chin et al.’s (2002) conversion algorithm), continent to the Korean peninsula and Japan were the fo- (b)GOCI-retrievedAOD(retrievedviatheYonseiaerosolretrieval cus of this study. However, defining the LRT events over algorithm (Lee et al., 2010)) and (c) assimilated AOD with two- Northeast Asia is not easy, mainly due to complexities in hour resolution over Northeast Asia at 09:00, 11:00, 13:00, and airmassmovements.Weconsideredlarge-scaleAODplumes 15:00LSTon10April2011. thatcausedthepeakAODvalueslargerthan0.4attherecep- tor sites (“peak AOD filter”). Such LRT AOD plumes were Engel-Coxetal.,2004;Liuetal.,2005;vanDonkelaaretal., further traced back via NOAA HYSPLIT (HYbrid Single- 2006;Choietal.,2009;Schaapetal.,2009;Tsaietal.,2011). Particle Lagrangian Integrated Trajectory) model analysis Several studies have estimated two-dimensional PM from (Draxler and Hess, 1998) from the points of time when the 10 the relationships between ground-based PM and satellite- peak AOD values occurred. The HYSPLIT model simula- 10 retrieved AOD (Wang and Christopher, 2003; Engel-Cox et tionswereperformedwithmeteorologicaldata,whichwere al., 2004; Liu et al., 2005; Schaap et al., 2009; Tsai et al., takenfromtheGDAS(GlobalDataAssimilationSystem)of 2011)ortheratiosofCTM-simulatedPM toAOD(Liuet NCEP. When the backward trajectories from the occurring 10 al.,2004;vanDonkelaaretal.,2006;Choietal.,2009). points of the peak AOD values had passed through China within48–72h,theAODplumeswerefinallydeterminedto be LRT plumes (“backward trajectory filter”). A LRT case 3 Resultsanddiscussions shown in Fig. 3 was decided by using both of the filters. Forexample,72hHYSPLITbackwardtrajectoryanalysisat The hourly assimilated AOD data was used to identify and three AERONET receptor sites in Korea for the LRT case analyze the PM LRT events over Northeast Asia. Based on in Fig. 3 is presented in Fig. 4. As shown, all the backward this,thevariationsoftheAODvaluesduringLRTeventsin trajectories were passed through China. By contrast, Fig. 5 comparisonwiththoseduringnon-LRTeventswereanalyzed showsanexampleofanon-LRTcase.BoththeLRTandnon- onamorequantitativebasis. LRTcaseswillbediscussedfurtherinSect.3.1. In order to investigate the LRT of particulate matter over 3.1 Long-rangetransportofaerosolsfromChinato Northeast Asia, the AOD values instead of PM concentra- Korea tionswereused.Inotherwords,theAODhasbeenregarded asaproxyquantityforPMconcentrationinthisstudy.Inthis A representative snapshot of an LRT event of particulate context, relationships between PM10 (or PM2.5) and AOD matter from China to the Korean peninsula, Japan, and the can be important. The relationships are affected by various northwestern Pacific Ocean is presented in Fig. 3. It can parameters, such as height of the PBL (planetary boundary be seen that a huge AOD plume (AOD>0.6) was gener- layer), RH, vertical distribution of aerosols, seasonality, di- ated in the greater Beijing area and Shandong province on urnalvariation, geographical information,particlecomposi- 10Aprilandwasthentransportedoverlongdistancestothe tions, and size distributions (Wang and Christopher, 2003; Korean peninsula following a low pressure trough. GOCI www.atmos-chem-phys.net/14/659/2014/ Atmos.Chem.Phys.,14,659–674,2014 666 M.E.Parketal.:Transboundaryparticulatepollution Backward trajectories (a) CMAQ AOD (b) GOCI AOD (c) Assimilated AOD 120E 130E 140E 120E 130E 140E 120E 130E 140E 120E 130E 140E 00 45N 45N 45N 45N 9:00 45N 04/12 09: 25N35N 25N35N 25N35N 25N35N 0 N N N N N 10 35 1:00 45 45 45 45 04/ 4/12 1 35N 35N 35N 35N N 0 N N N N 5 25 25 25 25 2 N N N N 5N 13:00 45N 45N 45N 45N 0 4 12 35 35 35 35 0 4/ 11: N 0 25N 25N 25N 25N 4/10 35 15:00 45NN 45NN 45NN 45NN 0 12 35 35 35 35 N 4/ 25 0 25N 25N 25N 25N 120E 130E 140E 120E 130E 140E 120E 130E 140E N 0.0 0.3 0.6 0.9 1.2 1.5 5 4 0 0 Fig.5.AsFig.3,foranon-LRTeventon12April2011.Thiscase : 3 was determined as non-LRT because the main AOD plumes were 1 N 0 5 transportedintoovernorthwesternPacificOcean,notovertheKo- 1 3 4/ reanpeninsulaand/orJapan. 0 N 5 2 N ilated AOD fields are much improved in comparison to the 5 4 predicted (a priori) CMAQ AOD distributions (first column 0 0 ofFig.3).TheaprioriCMAQAODvalueshaveatendency : 5 1 N tobeunderestimatedcomparedtotheGOCI-retrievedAOD 10 35 values,asshowninFig.3.Thisunderestimationisbelieved 4/ toberelatedtouncertaintiesintheemissionratesofgaseous 0 N andparticulatepollutantsandtheCMAQmodelsimulations, 5 2 as well as the uncertainties in the assumptions made during 120E 130E 140E theAODestimationfromtheCMAQmodelingresults. Fig.4.NOAAHYSPLIT72hbackwardtrajectoryanalysisatthree In this analysis, the AOD calculation via Chin et KoreanAERONETsites(Baengnyeong,Yonsei_Univ(Seoul),and al.’s (2002) conversion method was used. However, sev- Gwangju_GIST) with 2h resolution at 09:00, 11:00, 13:00, and eral other estimations were also tested (e.g., Malm et al., 15:00LSTon10April2011. 1994; Chin et al., 2004; Park et al., 2011). One example is shown in Fig. 6 and Table 3, which were produced by Parketal.’s(2011)conversionmethod.Itwasfoundthatthe retrievals with one-hour intervals from 09:00 to 16:00LST AOD values were underestimated because the MEE values (eightsnapshotsperday)on10Aprilshowhighaerosolload- and hygroscopic enhancement factor (fij(RH)) of Park et ings(AOD>1.2)overtheShandongpeninsulaandShanghai al.’s (2011) conversion method were reported to be in gen- regions that extend over Korea. The plumes extend farther eralsmallerthanthoseofChinetal.’s(2002)method.After outovertheYellowSeaandslowlyshifttolowerlatitudesas assimilationboththemagnitudesandspatialdistributionsare time progresses. In Fig. 3, only two-hour resolution results significantlyimproved.TheAODLRTeventshowninFig.3 are presented. It is important to note that GOCI AOD val- isonlyanexample.Seventofourteensmall-andlarge-scale uesarenotretrievedinregionswherecloudsexist.Asshown AODLRTeventsoccurredoverthetwo-monthperiod(from inFig.3,cloud-contaminatedpixelsappearwhite,whichin- 1Aprilto31May2011). dicates that no data is available at these pixels. The GOCI Furthermore, the non-LRT events were also identified. retrievals,whenassimilatedintotheCMAQmodel,produce During the non-LRT periods, air masses were generally completespatialdistributionswhereAODisestimatedinall stationary.Althoughtheinfluxofairpollutantsemittedfrom pixels(seethethirdcolumnofFig.3).Therefore,theassim- the highly polluted China regions to the Korean peninsula Atmos.Chem.Phys.,14,659–674,2014 www.atmos-chem-phys.net/14/659/2014/ M.E.Parketal.:Transboundaryparticulatepollution 667 Table3.ComparisonanalysisoftheassimilatedAODforLRTandnon-LRTeventsatfiveAERONETsitesduringtheentiremodelingperiod of1Aprilto31May2011. Non-LRTevents LRTevents Datafractionof AODincrease RatioofAODincrease LRTevents duringLRT duringLRT (xLRTinEq.8) events3 events4 N1 σ2 Avg. Max. N σ Avg. Max. Baengnyeong 849 0.11 0.16 0.95 606 0.36 0.59 2.15 0.42 0.43 2.59 Yonsei_Univ(Seoul) 821 0.15 0.22 0.77 634 0.29 0.49 2.13 0.44 0.28 1.28 Gwangju_GIST 1024 0.13 0.20 1.10 431 0.31 0.47 1.89 0.30 0.27 1.36 Gosan_SNU 967 0.12 0.17 1.09 488 0.24 0.41 1.53 0.34 0.24 1.37 Osaka 1247 0.11 0.16 1.16 208 0.21 0.39 1.23 0.14 0.23 1.41 Total 0.12 0.18 1.16 0.31 0.49 2.15 0.33 0.31 1.68 ThecalculationswereconductedwiththeassimilatedAODproducts.TheAODdataassimilationswerecarriedoutwiththeGOCI-retrievedAODproducts(retrievedviatheYonseialgorithm(Leeet al.,2010))andtheCMAQ-simulatedAODproducts(calculatedviaParketal.’sconversionalgorithm(Parketal.,2011)). 1Thenumberofdatafornon-LRTorLRTeventsfortheentiremodelingperiod; 2standarddeviation; 3AODincreasedbyLRTeventsabovetheaveragebackgroundAODcalculatedduringnon-LRTperiods; 4theratioswereestimatedby((AODLRT−AODnon-LRT)/AODnon-LRT).Here,AODLRTandAODnon-LRTindicatetheaverageAODcalculatedduringtheLRTandnon-LRTevents,respectively. Table4.ComparisonanalysisoftheassimilatedAODforLRTandnon-LRTeventsatfiveAERONETsitesduringtheentiremodelingperiod of1Aprilto31May2011. Non-LRTevents LRTevents Datafractionof AODincrease RatioofAODincrease LRTevents duringLRT duringLRT (xLRTinEq.8) events3 events4 N1 σ2 Avg. Max. N σ Avg. Max. Baengnyeong 849 0.12 0.22 0.98 606 0.48 0.79 2.79 0.42 0.57 2.65 Yonsei_Univ(Seoul) 821 0.21 0.30 1.13 634 0.37 0.66 2.93 0.44 0.35 1.17 Gwangju_GIST 1024 0.16 0.27 1.22 431 0.40 0.63 2.50 0.30 0.36 1.30 Gosan_SNU 967 0.12 0.22 1.14 488 0.31 0.54 1.95 0.34 0.32 1.47 Osaka 1247 0.11 0.21 0.90 208 0.22 0.48 1.26 0.14 0.27 1.27 Total 0.15 0.24 1.22 0.40 0.65 2.93 0.33 0.40 1.67 ThecalculationswereconductedwiththeassimilatedAODproducts.TheAODdataassimilationswerecarriedoutwiththeGOCI-retrievedAODproducts(retrievedviatheYonseialgorithm(Leeet al.,2010))andtheCMAQ-simulatedAODproducts(calculatedviaChinetal.’sconversionalgorithm(Chinetal.,2002)). 1Thenumberofdatafornon-LRTorLRTeventsfortheentiremodelingperiod; 2standarddeviation; 3AODincreasedbyLRTeventsabovetheaveragebackgroundAODcalculatedduringnon-LRTperiods; 4theratioswereestimatedby((AODLRT−AODnon-LRT)/AODnon-LRT).Here,AODLRTandAODnon-LRTindicatetheaverageAODcalculatedduringtheLRTandnon-LRTevents,respectively. and Japan was significantly reduced, the stagnant weather caseswerealsointroducedbyAl-Saadietal.(2005)withthe conditions could seriously deteriorate air quality. Figure 5 MODISAODdataovertheUnitedStates.Anotherpossibil- shows a case of the non-LRT events. Noticeable aerosol ityforthisplumeisthataerosolscouldbegeneratedthrough plumesdirectlytransportedfromChinatotheKoreanpenin- Siberian forest fires. In order to check this possibility, the sula and Japan could not be identified. Some AOD plumes global MOZART (Model for OZone And Related chemi- weregeneratedinthesouthernpartsofChina,andwerethen cal Tracers) model simulation data was investigated (http: transported over the northwestern Pacific Ocean. This case //www.acd.ucar.edu/wrf-chem). But no Siberian fire signif- wasclassifiedasnon-LRTcasesincetheAODplumeswere icantlyaffectedaerosolplumeson/before12April2011. notdirectlytransportedtotheKoreanpeninsulaand/orJapan. The AOD LRT events were investigated at the five In addition, a high AOD plume (in the second column AERONET sites (Holben et al., 1998) in the Korean penin- in Fig. 5) was transported through southern Russia (be- sula and in Japan shown in Fig. 1. The AERONET AOD tween09:00and11:00LST).Thisplumeappearstobethin values observed at ground sites are regarded as “ground clouds (i.e., cloud optical depth (COD)). This can be con- truth”becausethesurfacereflectancedoesnotinterferewith firmed partly via the Terra/MODIS AOD data at 10:30LST them (Holben et al., 1998; Dubovik et al., 2000; Chin et on 12 April. The Terra/MODIS AOD data did not show al., 2002, 2004; Park et al., 2011), and due to the high ac- any AOD plume over the same region (refer to the third curacy (∼0.01–0.02) of the fully calibrated data (Eck et and the fourth rows in Fig. 2). Since the GOCI AOD algo- al., 1999). Figure 7 shows the comparison of the GOCI- rithm has limitations in completely eliminating clouds, thin retrieved/assimilatedAODproducts(redhorizontalbarsand clouds are sometimes considered aerosol plumes. Similar blue solid line in Fig. 7, respectively) with the AERONET www.atmos-chem-phys.net/14/659/2014/ Atmos.Chem.Phys.,14,659–674,2014 668 M.E.Parketal.:Transboundaryparticulatepollution timatedfromEq.(7)(greybars)inFig.8.Asshown,thereare (a) CMAQ AOD (b) GOCI AOD (c) Assimilated AOD 120E 130E 140E 120E 130E 140E 120E 130E 140E reasonableagreementsbetweenthetwoPM concentrations N N N N 10 00 45 45 45 45 over two-month periods, except for several time windows 09: N N N N such as 9–11 April and 13–17 May. This example (Fig. 8) 10 35 35 35 35 04/ 25N 25N 25N 25N issurpfarecseePntMedcohnerceenitnraotirodnesr.tAoltshhoouwghhroewasoAnOaDbleisagrreeleamtedenttos N N N N 00 45 45 45 45 betweentheobservedandestimatedPMconcentrationswere 1: 4/10 1 35N 35N 35N 35N sdheovwelnopiendFinigo.r8d,erthteocmoonrveearscicounramteeltyhcoodnsvsehrotuAlOdDbetofuPrMth1e0r 0 25N 25N 25N 25N (or PM2.5) over East Asia, with the consideration of more 00 45N 45N 45N 45N factors,suchasheightofPBL,RH,andpresenceofdustand 13: N N N N BB plumes in the free troposphere (Wang and Christopher, 4/10 35 35 35 35 2003; Engel-Cox et al., 2004; Liu et al., 2005; van Donke- 0 N N N N 25 25 25 25 laaretal.,2006;Choietal.,2009;Schaapetal.,2009;Tsai 00 45N 45N 45N 45N etal.,2011). 5: 10 1 35N 35N 35N 35N 3.2 Estimationoftheimpactsoflong-rangetransport 4/ 0 N N N N 25 25 25 25 120E 130E 140E 120E 130E 140E 120E 130E 140E Thegrey-shadedareasinFig.7representtheperiodsduring 0.0 0.3 0.6 0.9 1.2 1.5 which the receptors were affected by the PM LRT events. ThePMLRTeventsweredeterminedbasedonthemeteoro- Fig. 6. As Fig. 3, except that the CMAQ-simulated AOD values logicalfieldsgeneratedfromMM5simulationstogetherwith werecalculatedviaParketal.(2011)’sconversionalgorithm. comprehensive backward trajectory analysis. For example, the Baengnyeong site was affected by the small- and large- AOD data (black bars in Fig. 7). The GOCI-retrieved AOD scaleLRTeventsfourteentimesoverthetwo-monthperiod. valuesagreewellwiththeAERONETvalues(e.g.,R=0.84, Mostofthehigh(andwide)AODpeaksareduetothelarge- see Table 5). However, both AERONET and GOCI data scale LRT events from China, and most of the small/sharp show large time periods with no retrievals, which points spikes are usually caused by local pollution under stagnant to the need for models to provide additional information. meteorologicalconditions.Thegrey-shadedperiodsinFig.7 The assimilated AOD product is well correlated with the usuallystartandendwhenthelarge-scaleLRTAODplumes AERONET and GOCI-retrieved AOD values and is much arriveinanddepartfromtheAERONETsites. more accurate than the a priori CMAQ AOD product when The background average AOD values (calculated exclud- comparedwiththeAERONETAODvalues.Thissituationis ing the AOD values during the LRT events) are represented summarizedinTable5,wheretheerrorsandbiasesafterthe by dashed lines at the five AERONET sites in Fig. 7. The assimilationbecomemuchsmallerthanthosebeforetheas- average impact of the transboundary PM pollution over the similation, indicating that the assimilation clearly improves entiretwo-monthperiod(i.e.,over“thenon-LRT+LRTpe- the quality of the AOD products. The assimilated product riods”) was calculated using the following formula over the providesacontinuousestimateofthetimeseriesofAODat two-monthperiod: everylocation,whichtheobservationsalonecannot(thered (cid:8) horizontalbarsinFig.7onlycoverlimitedtimeperiods). AODavg= Ni=1{AODLRT×xLRT+NAODnon-LRT×(1−xLRT)}, (8) As discussed previously, the AOD values are related to surface PM concentrations. Figure 8 shows an example of how to estimate the surface PM concentrations from the AOD =(cid:6)AOD=AOD −AOD , (9) assimilated AOD values. The daily averaged AOD values inc LRT non-LRT ((AOD)assimilated)showninFig.7wereconvertedintoPM10 whereAODavg,AODnon-LRT,andAODLRT representtheav- ((PM10)estimated) at five AERONET sites, using following erage AOD values during the entire period and the average proportionalrelationship(vanDonkelaaretal.,2006): AOD values calculated during the non-LRT and LRT peri- (cid:6) (cid:7) ods,respectively.x isthefractionoftheLRTeventsover PM LRT (PM10)estimated= 10 ×(AOD)assimilated. (7) thetwo-monthperiod.N isthetotalnumberofthegridcells AOD simulated being considered (for the calculation at an AERONET site, Twenty-four hour PM was also measured simultaneously N =1).Afterthat,theaverageAODincrease(AOD )dur- 10 inc at three Korean AERONET locations by the Korean Na- ingthetwo-monthperiodwascalculatedbyEq.(9).There- tionalInstitute ofEnvironmental Research(NIER). Theob- sultsfortheanalysisfortheAERONETsitesaresummarized served24hPM concentrations(blackdots)werethenplot- inTable4.Fromthisanalysis,theaverageAODincreaseof 10 tedtogetherwiththedailyaveragedPM concentrationses- 117–265%isfoundatthefiveAERONETsites. 10 Atmos.Chem.Phys.,14,659–674,2014 www.atmos-chem-phys.net/14/659/2014/

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