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NO2 remote sensing from APEX PDF

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Atmos.Meas.Tech.Discuss.,5,2449–2486,2012 Atmospheric Dis www.atmos-meas-tech-discuss.net/5/2449/2012/ Measurement c AMTD u doi:10.5194/amtd-5-2449-2012 Techniques s s ©Author(s)2012.CCAttribution3.0License. Discussions io 5,2449–2486,2012 n P a p Thisdiscussionpaperis/hasbeenunderreviewforthejournalAtmosphericMeasurement e NO remote sensing r 2 Techniques(AMT).PleaserefertothecorrespondingfinalpaperinAMTifavailable. from APEX | D C.Poppetal. is c High resolution NO remote sensing from u s 2 s io the Airborne Prism EXperiment (APEX) n TitlePage P a p Abstract Introduction imaging spectrometer e r Conclusions References | C. Popp1, D. Brunner1, A. Damm2, M. Van Roozendael3, C. Fayt3, and D Tables Figures is B. Buchmann1 c u ss J I 1Empa,SwissFederalLaboratoriesforMaterialsScienceandTechnology, io n 8600Du¨bendorf,Switzerland P J I 2RemoteSensingLaboratories,UniversityofZurich,Winterthurerstrasse190, ap e 8057Zurich,Switzerland r Back Close 3BelgianInsituteforSpaceAeronomy(BIRA-IASB),AvenueCirculaire3, | FullScreen/Esc 1180Brussels,Belgium D Received: 1March2012–Accepted: 19March2012–Published: 28March2012 isc Printer-friendlyVersion u s Correspondenceto: C.Popp([email protected]) s io InteractiveDiscussion n PublishedbyCopernicusPublicationsonbehalfoftheEuropeanGeosciencesUnion. P a p e r 2449 | Abstract D is c AMTD u We present and evaluate the retrieval of high spatial resolution maps of NO vertical s 2 s column densities (VCD) from the Airborne Prism EXperiment (APEX) imaging spec- ion 5,2449–2486,2012 trometer. APEX is a novel instrument providing airborne measurements of unique P a p 5 spectral and spatial resolution and coverage as well as high signal stability. In this er NO2 remote sensing study,weusespectrometerdataacquiredoverZurich,Switzerland,inthemorningand from APEX | lateafternoonduringaflightcampaignonacloud-freesummerdayinJune2010. NO 2 VCD are derived with a two-step approach usually applied to satellite NO retrievals, D C.Poppetal. 2 is i.e.aDOASanalysisfollowedbyairmassfactorcalculationsbasedonradiativetransfer c u s computations. s 10 io Our analysis demonstrates that APEX is clearly sensitive to NO VCD above typi- n TitlePage 2 P cal European tropospheric background abundances (>1×1015moleccm−2). The two- a p Abstract Introduction e dimensional maps of NO2 VCD reveal a very plausible spatial distribution with strong r gradientsaroundmajorNO sources(e.g.Zurichairport,wasteincinerator,motorways) Conclusions References x | andlowNO inremoteareas. ThemorningoverflightsresultedingenerallyhigherNO 15 2 2 D Tables Figures VCDandamoredistinctpatternthantheafternoonoverflightswhichcanbeattributed is c to the meteorological conditions prevailing during that day (development of the bound- u ss J I ary layer and increased wind speed in the afternoon) as well as to photochemical loss io n of NO2. The remotely sensed NO2 VCD are also highly correlated with ground-based P J I 20 in-situ measurements from local and national air quality networks (R=0.73). Airborne ap e NO remote sensing using APEX will be valuable to detect NO emission sources, to r Back Close 2 2 provide input for NO2 emission modeling, and to establish links between in-situ mea- | FullScreen/Esc surements, air quality models, and satellite NO products. 2 D is c Printer-friendlyVersion u s 1 Introduction s io InteractiveDiscussion n P 25 Nitrogen dioxide (NO2) is an important reactive trace gas in the troposphere. NO2 ap acts as an ozone and aerosol precursor and can directly or indirectly affect human e r 2450 | health (e.g. pulmonary or cardiovascular diseases) (Brunekreef and Holgate, 2002) D is and ecosystem functions and services (e.g. damage of leaves, reduction of crop pro- c AMTD u s duction, acidification) (Bell and Treshow, 2002). Besides natural sources such as s io 5,2449–2486,2012 lightning and soil emissions the major fraction of tropospheric NO is related to an- n 2 P thropogenic activities, notably fossil fuel combustion by traffic and industry. Despite a 5 p significant improvements of air quality in European countries during the past two e NO remote sensing r 2 decades, air quality thresholds are still frequently exceeded and further efforts are from APEX | neededparticularlyregardingreductionsofparticulatematter,ozone,andnitrogenox- ides (NOx=NO+NO2). Measurements of NO2 in the troposphere are performed with Dis C.Poppetal. c various in-situ, airborne, and spaceborne instruments. Tropospheric vertical column u 10 s densities (TVCD) retrieved from satellites (e.g. from the Scanning Imaging Absorp- sio n TitlePage tion Spectrometer for Atmospheric Chartography (SCIAMACHY), the Global Ozone P Monitoring Experiment (GOME(-2)), or the Ozone Monitoring Instrument (OMI)) have a p Abstract Introduction e largely contributed to a better understanding of the global distribution of NO as well r 2 as its sources and trends (e.g. Boersma et al., 2004; Richter et al., 2005; van der A Conclusions References 15 | et al., 2008; Zhou et al., 2012). The spatial resolution of satellite products in the order D Tables Figures of multiple tens of kilometers is only sufficient to detect aggregate sources like entire is c cities(Beirleetal.,2011)andindividualsourceslikeemissionsfrompowerplants(Kim uss J I etal.,2006)orships(Beirleetal.,2004)iftheyaresufficientlyseparatedinspacefrom io n 20 other sources. Ground-based in-situ instruments, on the other hand, provide accu- P J I a rate and continuous trace gas measurements but lack of homogeneous geographical p e coverage. Airborne remote sensing observations can in this regard provide a valuable r Back Close link between ground-based and spaceborne NO2 information. For example, airborne | FullScreen/Esc multi-axis differential optical absorption spectroscopy (AMAXDOAS) was used to re- D 25 trieve NO2 TVCD (Wang et al., 2005), NO2 profile information (Bruns et al., 2006), or iscu Printer-friendlyVersion to validate SCIAMACHY NO TVCD (Heue et al., 2005). Heue et al. (2008) demon- s 2 s strated the capability of an imaging DOAS instrument to retrieve two dimensional NO io InteractiveDiscussion 2 n distributions over the highly polluted Highveld plateau in South Africa. P a p e r 2451 | The Airborne Prism EXperiment (APEX) imaging spectrometer is a state-of-the art D is instrument with an unprecedented combination of high spectral and spatial resolution, c AMTD u s good two dimensional geographical coverage, and high signal stability. Two NO dis- s 2 io 5,2449–2486,2012 tribution maps were retrieved from imaging spectrometer data acquired over Zurich, n P Switzerland, in the morning and the late afternoon of 26 June 2010. Our results are a 5 p considered as one of the first spatio-temporal investigations of the NO distribution on e NO remote sensing 2 r 2 aregionaltolocalscale. Inparticular,wepresentthefirsthighresolutionmapsofNO from APEX 2 | VCD in a city measured by an airborne imaging spectrometer. The specific objectives D C.Poppetal. ofthisstudyare(i)thepresentationofaretrievalschemetoobtainNO2 quantitiesfrom is c APEX imaging spectrometry data and (ii) the qualitative and quantitative assessment u 10 s of the NO2 products, considering amongst others in-situ measurements of NO2. sio n TitlePage P a p Abstract Introduction 2 Instrument and data acquisition e r Conclusions References 2.1 The APEX instrument | D Tables Figures APEX is a dispersive pushbroom imaging spectrometer for environmental monitoring is c u 15 developedbyaSwiss-BelgiumconsortiumintheframeworkoftheESA-PRODEXpro- ss J I gramme (Itten et al., 2008). APEX consists of the imaging spectrometer itself, a Cali- io n brationHomeBase(CHB)forinstrumentcalibration,andadataProcessingandArchiv- P J I a ing Facility (PAF) for operational product generation (Jehle et al., 2010). Table 1 gives pe r Back Close a brief overview of the sensor characteristics. TheAPEXimagingspectrometerconsistsofaCCDdetectorforthevisibleandnear | FullScreen/Esc 20 infrared (VNIR) and a CMOS detector for the shortwave infrared (SWIR) wavelength D is region. TheNO retrievalisbasedonabsorptionbandsintheUV/VISspectraldomain c Printer-friendlyVersion 2 u s and, hence, only the VNIR specification is discussed hereinafter. Since atmospheric s io InteractiveDiscussion trace gases exhibit spectrally narrow absorption features, the (spectrally) unbinned n P 25 configurationwasappliedtoprovidehighestspectralresolution. Thespectralsampling a p interval (SSI) and the full width half maximum (FWHM) are non-linear functions of e r 2452 | the wavelength and increase with longer wavelengths. According to pre-flight sensor D is calibration, the SSI increases from 0.63 to 1.44nm and the FWHM from 0.83 to 1.66 c AMTD u s between 420nm and 520nm where NO slant column densities (SCD) are usually s 2 io 5,2449–2486,2012 derived. APEXisapushbroomscannerandmeasuresradiancesin1000spatialpixels n P across-track. The extent of the flight line along-track depends on the pre-defined flight a 5 p pattern. The spatial resolution in across-track direction is determined by the sensor’s e NO remote sensing r 2 instantaneousfieldofview(IFOV)of0.028◦. Thespatialresolutionalong-trackdepends from APEX | on the integration time. This unparalleled combination of high resolution, geographical D C.Poppetal. coverage, and high signal stability makes APEX very attractive for a range of remote is c sensing applications, e.g. in the fields of vegetation, atmosphere, limnology, geology, u 10 s or natural hazard studies. sio n TitlePage P 2.2 Test site and data a p Abstract Introduction e r Within the APEX acceptance flight campaign in 2010, extensive data acquisition ac- Conclusions References | tivities took place over Belgium and Switzerland. Six of these image data sets were acquiredinunbinnedmodeoverZurich,Switzerland,onSaturday26June(c.f.Fig.1). D Tables Figures 15 is Three of them were flown around 10:00 local time (08:00UTC) and three in the late cu afternoon around 17:30 local time (15:30UTC). The data was acquired approximately ss J I io 5000mabovegroundwithanintegrationtimeof57ms,leadingtoapixelsizeofabout n P J I 2.5macross-trackandapproximately6malong-track,respectively. Theentiredaywas a p 20 cloud-free. er Back Close Zurich is Switzerland’s largest city with nearly 400000 inhabitants surrounded by | FullScreen/Esc an agglomeration of more than one million inhabitants. The test site includes a wide D range of surface types like buildings, roads, parks, forests, and part of Lake Zurich is c Printer-friendlyVersion (Fig. 1, c.f. also APEX true color composite in Fig. 7a). It also includes more rural u s s 25 areas with decreased atmospheric pollution levels like the Uetliberg mountain range. io InteractiveDiscussion n SeveralmajorNO sourceswerecovered. Threenationalmotorwayssurroundthecity x P a to the north, west and south (A1, A3, A4) and major transit roads lead through the city p e with a usually high traffic volume. In addition, two waste incinerators as well as part r 2453 | of the approach corridor of Zurich airport are located in the test site area. Zurich was D is also selected for the flight experiments because of the dense ground-based air quality c AMTD u s networkwitheightstationswithintherangecoveredbyAPEX(Fig.1). TheNationalAir s io 5,2449–2486,2012 Pollution Monitoring Network (NABEL) provides half-hourly averaged measurements n P of classical air pollutants like NO , O , SO , PM at Zurich Kaserne (urban back- a 5 2 3 2 10 p ground, situated in a park near the city center) and Duebendorf (suburban). Additional e NO remote sensing r 2 air quality measurements and meteorological parameters are available from the inter- from APEX | cantonal network Ostluft which maintains eight sites in the area of interest from which D C.Poppetal. six sites provided data for 26 June 2010: Heubeeribuehl (periphery), Wettswil Filderen is c (rural,closetomotorway),WettswilWeieracher(rural),Stampfenbach(urban,kerbside, u 10 s moderate traffic), Schimmelstrasse (urban kerbside, high traffic volume), and Opfikon sio n TitlePage (kerbside, motorway). P a p Abstract Introduction 2.3 Data preparation e r Conclusions References | APEX data were acquired in unbinned mode to provide highest spectral resolution. Thisinstrumentalsetting,however,isattheexpenseofthesignalstability. Toincrease D Tables Figures 15 is the signal-to-noise (SNR) ratio, the imaging spectrometer data were spatially aggre- cu gated. Aboxsizeof20×20pixelswasappliedwhichisexpectedtoincreasetheSNR ss J I √ io twenty times (or 400) assuming uncorrelated noise. An image based SNR estima- n P J I tionappliedontheoriginalunbinnedAPEXdatarevealedaSNRof158.5at490nmfor a p 20 darksurfaces(water). Spatialaggregation,hence,increasestheSNRtoapproximately er Back Close 3170 for dark surfaces. It is relevant to note that image based SNR estimates usually | FullScreen/Esc overestimate noise or underestimate the SNR respectively, as surface variability is in- D herent in the image statistics. The spatial averaging resulted in a decreased pixel size is of around 50×120m2. cu Printer-friendlyVersion s s 25 The APEX spectrometer is spectrally and radiometrically calibrated pre-flight. How- io InteractiveDiscussion ever,itisworthmentioningthatthiscalibrationdoesnotcompensateforcertaineffects n P occurring in-flight. For example, pushbroom sensors are typically affected by slight ap e spectral miss-registrations across-track, e.g spectral smile effects (D’Odorico et al., r 2454 | 2010) which may depend on the specific flight conditions. In order to minimize these D is effects, the NO retrieval was performed on geometrically uncorrected data to allow a c AMTD 2 u s scan-raw wise processing of the data. In addition, NO is determined from raw data s 2 io 5,2449–2486,2012 (digital numbers or DN) and a spectral calibration is performed directly as part of the n P retrieval algorithm to account for spectral effects under flight conditions (c.f. Sect. 3.1). a 5 p In order to obtain surface reflectance as an important input parameter of the re- e NO remote sensing r 2 trieval algorithm a software binning was applied to transform the unbinned data from APEX | to the standard binning pattern and the data were subsequently calibrated to at- D C.Poppetal. sensor radiance using the APEX-PAF. The re-binned radiance data were then at- is c mospherically corrected using the ACTOR-4 software tool (Richter and Schla¨pfer, u 10 s 2002) to obtain Hemispherical-Conical-Reflectance (HCRF) data. In a last step, the sio n TitlePage unbinned and binned APEX data were geometrically corrected using the PARGE P orthorectification software (Schla¨pfer and Richter, 2002). This processing step is a p Abstract Introduction e needed to re-project auxiliary data (e.g. a digital elevation model (DHM25, http://www. r swisstopo.admin.ch/internet/swisstopo/en/home/products/height/dhm25.html, last ac- Conclusions References 15 | cess:12March2012))totherawgeometryoftheAPEXdatatoallowascan-rawwise D Tables Figures processing as mentioned before. Further, the geocorrected data is essential to re- is c late the APEX NO2 vertical column density (VCD) to the in-situ measurements of NO2 uss J I concentrations and to identify objects of interest like large NO point sources. io x n P J I a 3 NO retrieval p 20 2 er Back Close The derivation of NO maps from APEX follows the two step approach usually applied 2 | FullScreen/Esc to satellite NO retrievals. In a first step, differential slant column densities (dSCD) are 2 D derived by the well known differential optical absorption spectroscopy (DOAS) tech- is c Printer-friendlyVersion nique(PlattandStutz,2008). Subsequently,thedSCDareconvertedtoVCDbymeans u s s 25 of air mass factors (AMF) calculated with a radiative transfer model. Detailed informa- io InteractiveDiscussion n tion about the physical principles, applications, and accuracies of DOAS and AMF P a computationscanbefoundelsewhere(Palmeretal.,2001;Boersmaetal.,2004;Platt p e and Stutz, 2008). r 2455 | 3.1 DOAS analysis D is c AMTD u Differential slant column densities (dSCD) were derived with the QDOAS software s s io 5,2449–2486,2012 (http://uv-vis.aeronomie.be/software/QDOAS/,lastaccess:12March2012,Faytetal., n 2011). DOAS analysis requires reference spectra which we obtained from the imag- P a p 5 ing spectrometer data themselves. Reference spectra were selected for each individ- er NO2 remote sensing ual (aggregated) flight column (along-track) to account for and minimize errors in the from APEX | DOAS analysis due to spectral miss-calibration (e.g. spectral smile). For this purpose, ten (across-track) rows were chosen by visual inspection in a forested and elevated D C.Poppetal. is area to the south of the city (c.f. Fig. 7a) which is assumed to only contain a back- c u s ground abundance of NO (pollution free). Subsequently, the ten rows were averaged s 10 2 io in the columnar direction to increase the SNR of the reference spectra. This finally n TitlePage P resulted in 50 across-track reference spectra per flight. a p Abstract Introduction NO absorptioncrosssections(at293K,Voigtetal.,2002)weresubsequentlyfitted e 2 r tothedifferentialopticaldepthderivedfromtheAPEXmeasurementsandthereference Conclusions References | spectra. Spectrallyslowlyvaryingsignatures(e.g.fromaerosolsorsurfacereflectance) 15 D Tables Figures were accounted for by including a fifth-order polynomial in the fit and instrumental ef- is c fects such as dark current and/or straylight are dealt with in QDOAS by introducing an u offset spectrum. Inelastic Raman scattering was considered by a Ring cross section ssio J I n computed by QDOAS (c.f. Fayt et al., 2011) and the interference with O2-O2 was ac- P J I 20 counted for by fitting an appropriate absorption cross section (Hermans et al., 2002). ap e Smallest fitting errors were found by using the 470–510nm wavelength region (c.f. red r Back Close rectangle in Fig. 2). The usage of a window at shorter wavelengths (e.g. 420–470nm) | FullScreen/Esc leadtoincreasedfittingerrors,probablyduetothelowersignallevelsandhighernoise D (and therewith lower SNR). is c Printer-friendlyVersion u 25 Accurate wavelength calibration is an important prerequisite for the DOAS analysis. s s As indicated above, raw DN (digital number) data was used to keep the highest sensi- io InteractiveDiscussion n tivityofthemeasurementsfortheNO retrieval. Thespectralcalibrationwastherefore P 2 a performed with the QDOAS algorithm itself. A high resolution solar spectrum (Chance p e r 2456 | and Kurucz, 2010) was applied to obtain spectral calibration information which was D is subsequently used to convolve and shift the high resolution absorption cross sections c AMTD u s to the APEX specifications. Two exemplary (pre-processed) APEX spectra from the s io 5,2449–2486,2012 VNIR detector recorded over a residential and a remote vegetated area are illustrated n P inFig.2. Thecorrespondingslantcolumnfitofthepixelovertheresidentialareaispre- a 5 p sentedinFig.3whichalsogivesanimpressionofthesensor’sspectralresolution. The e NO remote sensing r 2 quality of the DOAS fit depends on the spectral and radiometric characteristics of the from APEX | instrument. The spectral calibration step in QDOAS disclosed some differences worth D C.Poppetal. mentioningtothepre-flightreportedAPEXspecifications(Sect.2.1andTable1)inthe is c 470–510nmwavelengthrange. TheDOASanalysisindicatedthattheindividualchan- u 10 s nels are positioned roughly 0.6nm higher than reported pre-flight and the (over wave- sio length) averaged across-track differences of their corrected position (spectral smile) is n TitlePage P ∼0.25nm. This is in line with recent findings from an in-flight and scene based APEX a p Abstract Introduction e performance assessment (D’Odorico et al., 2011). Furthermore, the QDOAS wave- r length calibration and slit function characterisation points to a FWHM about double Conclusions References 15 | the spectral resolution measured in the laboratories at the CHB. The reasons for this D Tables Figures discrepancy are not fully understood yet and further analysis is currently carried out. is c Finally,notethatnegativedSCDcanoccurwhentheSCDfromthereferencespectrum uss J I is larger than that from the fitted spectrum or due to noise. io n P J I 3.2 Air mass factor calculation a 20 p e r Back Close The AMF expresses the ratio between slant and vertical column of a trace gas: | FullScreen/Esc SCD=VCD×AMF (1) D is and is a measure of the average backscatter path through the atmosphere of the pho- c Printer-friendlyVersion u tons observed by the sensor. The AMF can be calculated as follows (Palmer et al., ss io InteractiveDiscussion 25 2001; Boersma et al., 2004): n P Pm (bˆ)x a AMF= L a,L (2) pe Px r a,L 2457 | where the subscript “L” denotes a specific atmospheric layer and m is the (box) air D L is mass factor per layer. Besides the layer subcolumns of the a priori NO profile (x ), c AMTD 2 a,L u s the AMF depends on forward model parameters (bˆ) such as the solar and viewing s io 5,2449–2486,2012 zenithandazimuthangles,surfacealbedo,aerosolextinctionprofile,andsurfacepres- n P sure. The box air mass factors were calculated using the Linearized Discrete Ordinate a 5 p Radiative Transfer model (LIDORT, Spurr, 2008): er NO2 remote sensing from APEX m =−1 ∂I (3) | L I ∂τ L D C.Poppetal. is where I is the intensity of the backscattered radiance and τ the optical depth of layer c L u “L”. ss io 10 With regard to radiative transfer computations, the surface albedo for every pixel n TitlePage P was derived from re-binned and atmospherically corrected APEX data themselves for a p Abstract Introduction the central wavelength of the fitting window (490nm). Surface height was taken from e r the digital elevation model DHM25 previously projected to the raw geometry of the Conclusions References | individual flight lines. Surface pressure for every pixel was subsequently obtained ap- plying the US Standard Atmosphere 1976 (http://www.pdas.com/coesa.html, last ac- D Tables Figures 15 is cess: 12 March 2012). The a priori NO2 profile was taken from the EURAD chemi- cu caltransportsimulations(http://www.eurad.uni-koeln.de/,lastaccess:12March2012) ss J I io over Switzerland at 5×5km2. The coarse resolution profile was subsequently scaled n P J I to the corresponding surface height of the aggregated APEX grid cell according to a p e 20 Zhou et al. (2009). Aerosol optical depth (AOD) at 500nm was taken from the Aerosol r Back Close Robotic Network (AERONET, Holben et al., 1998) site Laegeren which is within ap- | FullScreen/Esc proximately 20km from the city of Zurich. The AOD was converted to an extinction D profileforeverypixelassuminganexponentialdecreasewithheightandascaleheight is c Printer-friendlyVersion of two kilometers. The box air mass factors from three exemplary (aggregated) APEX u s s 25 pixels are depicted in Fig. 4. APEX’s sensitivity toward a NO2 signal is highest in the io InteractiveDiscussion n atmospheric layer below the aircraft (red horizontal line) and is decreasing toward the P a surfaceandtowardhigheratmosphericlayers. Amongalltheabovementionedparam- p e eters, the surface albedo has the largest impact on the AMF, e.g. the bright surface r 2458 |

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Interactive Discussion. Discussion Our analysis demonstrates that APEX is clearly sensitive to NO2 VCD above typi- Nitrogen dioxide (NO2) is an important reactive trace gas in the troposphere. Besides natural sources such as Pairs: Unconventional Absorbers of Radiation in the Atmosphere,
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