Atmos. Chem. Phys., 10, 7997–8009, 2010 www.atmos-chem-phys.net/10/7997/2010/ doi:10.5194/acp-10-7997-2010 © Author(s) 2010. CC Attribution 3.0 License. Atmospheric Chemistry and Physics Optical extinction by upper tropospheric/stratospheric aerosols and clouds: GOMOS observations for the period 2002–2008 F. Vanhellemont1 , D. Fussen1 , N. Mateshvili1 , C. Tétard1 , C. Bingen1 , E. Dekemper1 , N. Loodts1 , E. Kyrölä2 , V. Sofieva2 , J. Tamminen2 , A. Hauchecorne3 , J.-L. Bertaux3 , F. Dalaudier3 , L. Blanot3,4 , O. Fanton d’Andon4 , G. Barrot4 , M. Guirlet4 , T. Fehr5 , and L. Saavedra5 1 Belgian Institute for Space Aeronomy, Brussels, Belgium Meteorological Institute, Helsinki, Finland 3 Service d’Aéronomie du CNRS, Verrieres-le-Buisson, France 4 ACRI-ST, Sophia-Antipolis, France 5 ESA-ESRIN, Frascati, Italy 2 Finnish Received: 2 February 2010 – Published in Atmos. Chem. Phys. Discuss.: 26 April 2010 Revised: 18 August 2010 – Accepted: 24 August 2010 – Published: 27 August 2010 Abstract. Although the retrieval of aerosol extinction coefficients from satellite remote measurements is notoriously difficult (in comparison with gaseous species) due to the lack of typical spectral signatures, important information can be obtained. In this paper we present an overview of the current operational nighttime UV/Vis aerosol extinction profile results for the GOMOS star occultation instrument, spanning the period from August 2002 to May 2008. Some problems still remain, such as the ones associated with incomplete scintillation correction and the aerosol spectral law implementation, but good quality extinction values are obtained at a wavelength of 500 nm. Typical phenomena associated with atmospheric particulate matter in the Upper Troposphere/Lower Stratosphere (UTLS) are easily identified: Polar Stratospheric Clouds, tropical subvisual cirrus clouds, background stratospheric aerosols, and post-eruption volcanic aerosols (with their subsequent dispersion around the globe). For the first time, we show comparisons of GOMOS 500 nm particle extinction profiles with the ones of other satellite occultation instruments (SAGE II, SAGE III and POAM III), of which the good agreement lends credibility to the GOMOS data set. Yearly zonal statistics are presented for the entire period considered. Time series furthermore convincingly show an important new finding: the sensitivity of GOMOS to the sulfate input by moderate volcanic eruptions such as Manam (2005) and Soufrière Hills (2006). Finally, PSCs are well observed by GOMOS and a first qual- Correspondence to: F. Vanhellemont ([email protected]) itative analysis of the data agrees well with the theoretical PSC formation temperature. Therefore, the importance of the GOMOS aerosol/cloud extinction profile data set is clear: a long-term data record of PSCs, subvisual cirrus, and background and volcanic aerosols in the UTLS region, consisting of hundreds of thousands of altitude profiles with near-global coverage, with the potential to fill the aerosol/cloud extinction data gap left behind after the discontinuation of occultation instruments such as SAGE II, SAGE III and POAM III. 1 Introduction Upper tropospheric and stratospheric particles (whether liquid or solid) are intensively studied for a number of reasons that can be roughly summarized as follows: (1) they have an impact on the Earth radiative balance due to their optical properties, (2) they play a crucial role in heterogeneous chemistry, and (3) they provide information on the emission of precursor species from which they originate. Here, the word ’particles’ should be taken in its most general context: liquid or solid aerosols of submicron size, cloud droplets or crystals with sizes of tens or hundreds of microns, etc. From previous experiences with satellite occultation instruments, we know that a few particle types are commonly encountered in the measurements: stratospheric aerosols, tropical subvisual cirrus clouds and Polar Stratospheric Clouds (PSCs). The stratospheric aerosol layer (or Junge layer, named after its discoverer; see Junge et al., 1961) consists of liquid droplets composed of a mixture of sulphuric acid and water. The layer manifests itself in a pronounced way after Published by Copernicus Publications on behalf of the European Geosciences Union. 7998 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations major volcanic eruptions that are powerful enough to inject teragrams of SO2 into the stratosphere, such as the ones of Mount Pinatubo (the Philippines, 1991) or El Chichón (Mexico, 1982); see Robock (2000). After an oxidation process, sulfate aerosols are formed that are subsequently transported globally, depending on the latitude of the eruption. Eventually they are removed from the stratosphere, although this process can take years. Nevertheless, the last major eruption (Mount Pinatubo) dates already from 18 years ago, and the stratospheric aerosol layer returned to its “background” level around 1997. Since then, no significant trend is observed in data from SAGE II, balloon-borne instruments and lidars (Deshler et al., 2003, 2006), even when compared with volcanically quiet years such as 1979. These findings suggest a more or less stable input of sulphuric species in the stratosphere that maintain the background layer. Crutzen (1976) suggested carbonyl sulfide (OCS) as the major precursor gas, although this hypothesis has been challenged (see e.g. Chin and Davis (1995); Leung et al. (2002)). Very recently, increased anthropogenic SO2 emission by coal burning in China has been proposed as a possible origin for an upward trend in lidar measurements of stratospheric aerosols (Hofmann et al., 2009). A good overview of stratospheric aerosol science can be found in (SPARC, 2006). Polar Stratospheric Clouds have been investigated for over two decades now. The well-known classification scheme of PSCs was originally based on observations of backscatter and depolarization ratios with lidar instruments (Poole and McCormick, 1988). Type Ia particles are believed to be relatively large crystalline particles consisting of hydrates of HNO3 such as Nitric Acid Trihydrate (NAT) or Dihydrate (NAD). The smaller, liquid Type Ib particles consist of a supercooled ternary solution (STS) of HNO3 , H2 SO4 and H2 O. The crystalline Type II particles are formed of pure water ice. PSCs have a crucial role in the stratospheric ozone depletion process over the Arctic and Antarctic regions, because of (1) heterogeneous chemistry on the particle surface and (2) the denitrification of the atmosphere by the sedimentation of mainly Type Ia particles. Formation of PSCs is driven by temperature: Type Ia and Ib particles form below about 195 K, while the Type II ice crystals form at the ice frost point, about 188 to 190 K in the lower stratosphere. These cold temperatures are provided in the polar regions during local winter. A more detailed description of PSC formation can be found in the review paper of Zondlo et al. (2000). The so-called subvisual cirrus clouds are a fairly recent discovery for the obvious reason that they are optically thin and thus invisible from the ground (hence the name): an upper limit for the optical thickness of 0.03 at 694 nm is sometimes mentioned in the literature. Long optical pathlengths ensure that satellite occultation instruments such as SAGE II have detected them frequently (Wang et al., 1996). They are mainly found in the tropics and midlatitudes, around the tropopause altitude region (16–17 km). Much is still to be learned about the formation of these clouds, but Jensen et al. Atmos. Chem. Phys., 10, 7997–8009, 2010 (1996) proposed at least two mechanisms: (1) they originate from horizontal anvil-shaped outflows of large convective cumulonimbus clouds, and (2) from nucleation inside a humid layer that experiences slow uplift through the extremely cold region of the tropopause. Subvisual cirrus form cloud layers with a very large horizontal extent (hundreds of kilometers) but are at the same time very thin (smaller than 1 km). In recent years they received a lot of attention due to their possible role in the radiative balance of the atmosphere, their impact on ozone concentrations through heterogeneous chemistry (Solomon et al., 1997), and their role in the dehydration of air that enters the tropical lower stratosphere (Jensen et al., 1996). The Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument was primarily intended to deliver accurate altitude profiles of trace gas concentrations. These retrievals can be performed since each gas is detected by its specific spectral signature in the measured light intensity. Atmospheric particle populations pose a more challenging problem since the spectral shape is unknown, with the direct consequence that it is a priori impossible to find out which kind of particles are in the line of sight of the instrument. This is the reason why GOMOS delivers only one common product, perhaps somewhat misleadingly dubbed “aerosol extinction”. It should be understood that this data product currently embraces all above-mentioned types of aerosol and cloud particles (or indeed even any unknown extinction phenomenon with a smooth spectral dependence). However, the distinction will be made in this paper with the use of additional information, such as time of appearance/disappearance, geolocation and altitude. First results on GOMOS aerosol/cloud extinction profiles representing the year 2003 were previously published (Vanhellemont et al., 2005). The data discussed here span a much longer time period, from 2002 to 2008. Furthermore, a new data version was used, with as most important feature the use of a quadratic polynomial of wavelength as aerosol extinction model, while the previous model as described in (Vanhellemont et al., 2005) was oversimplified and consisted of a fixed inverse wavelength function. 2 GOMOS: Instrument and obtained data set The GOMOS instrument has been adequately described elsewhere (Kyrölä et al., 2004; Bertaux et al., 1991, 2000, 2010), so we only give a brief summary here. GOMOS, onboard ENVISAT, was launched in a sunsynchroneous orbit on 1 March 2002. GOMOS routine operations started in August 2002, and since then the instrument has been recording data almost continuously until present. GOMOS observes occultations of stars (chosen from a predefined catalogue) behind the earth limb, and records the received light intensity in the UV/Vis/NIR spectral range: 248–690 nm (spectrometers A1 and A2), 755–774 nm (spectrometer B1) and 926–954 nm www.atmos-chem-phys.net/10/7997/2010/ F. Vanhellemont et al.: GOMOS Aerosol/Cloud observations Vanhellemont et al.: GOMOS Aerosol/CloudExtinction Extinction observations 4 5 # occultations 1.5 1 0.5 2002 4 15 2004 2006 Year 0.5 2 10 5 0 −2 1 5 x 10 0 2 Star magnitude 4 3 1.5 0 −180 2008 −90 0 90 Longitude [degrees] 2 1 4 x 10 4 1 0.5 0 1 2 3 Star temperature [K] x 10 0 −90 180 1.5 0 7999 4 x 10 # occultations 0 # occultations 2 # occultations x 10 # occultations # occultations 2 3 4 4 x 10 −45 0 45 Latitude [degrees] 90 x 10 3 2 1 0 50 100 150 Solar zenith angle [degrees] Fig. 1. Occultation statistics for the entire GOMOS data set spanning the period August 2002 - May 2008. Shown are histograms representing the number of GOMOS occultations as functiondata of (from left to right, the top to bottom)August year, longitude, latitude, star magnitude, star histograms temperature representing Fig. 1. Occultation statistics for the entire GOMOS set spanning period 2002–May 2008. Shown are and solar zenith angle. Blueas histograms to the fraction occultations dark limb, red ones to the fraction in bright the number of GOMOS occultations functionrefer of (from left toofright, top to inbottom) year, longitude, latitude, starlimb. magnitude, star temperature and solar zenith angle. Blue histograms refer to the fraction of occultations in dark limb, red ones to the fraction in bright limb. ter sampling is obtained. The actual star spectrum is (in normal mode) calculated from 7 CCD rows of the spectrometers, to a field of view of signals, 0.01 degrees. (spectrometerequivalent B2). From measured transmittances It is important to know uncertainty on the obtained are calculated that in turn are usedthat tothe derive altitude concenprofiles tempertration profiles for Ois3largely , NO2determined , NO3 , H2by Othe andmagnitude O2 , andand temperature of the observed star. But even bright stars (such as Sirature profiles.ius) Furthermore, aerosol/cloud extinction are weak light sources in comparison with theprofiles Sun; proat different wavelengths are obtained. files obtained from stellar occultations have therefore larger uncertainties the ones from solar occultations. This disThe integration timethan to record a GOMOS full spectrum is however largely compensated for byby thethis fact is 0.5 s. Theadvantage actual vertical sampling is determined that stars are abundant in the sky: about 30 to 40 occultatime, togethertions with thebeen vertical velocity theorbit, tangent point have typically observedofper although this (between 0.5number and 3.4 km/s, depending on the obliquity thean decreased to 20 or 30 occultations per orbit of after instrument malfunction in optical 2005. Hundreds thousands occultation) and refraction of the path atoflower alti-of observed by GOMOS the start tudes (whichoccultations decreaseshave thebeen tangent point verticalsince velocity). of the mission. A maximum vertical sampling resolution of 1.7 km can be The occultation statistics for the period August 2002 - May expected, but2008 during very oblique occultations a 200 (a total of about 600,000 events, the entire datameter set that sampling is obtained. star ofspectrum is represented (in norwas availableThe to usactual at the time writing) are by histograms in 7Fig. 1. rows Of course, thespectrometers, lower number of mal mode) calculated from CCD of the for theof years and 2008 are caused by an equivalent tooccultations a field of view 0.012002 degrees. incomplete sampling of these years, while the smaller numIt is important know that the the obtained ber into2005 resulted fromuncertainty the instrumentonfailure mentioned profiles is largely by the magnitude temperearlier.determined Longitudinal sampling is clearly veryand homogeneous. Most occultations occur at midlatitudes, ature of the observed star. But even bright starsalthough (such plenty as Sir-of polar measurements are available. Most stars have ius) are weak light sources in comparison with the Sun;moderprofiles obtained from stellar occultations have therefore larger uncertainties than the ones from solar occultations. This disadvantage is however largely compensated for by the fact that stars are abundant in the sky: about 30 to 40 occultations have been typically observed per orbit, although this number decreased to 20 or 30 occultations per orbit after an instrument malfunction in 2005. Hundreds of thousands of occultations have been observed by GOMOS since the start of the mission. www.atmos-chem-phys.net/10/7997/2010/ ate to weak brightness, and are rather cold. Also, about half of the occultations occur in the Sun-illuminated atmosphere (‘bright Solar Zenith Angle SZA the other half 2002 - May Thelimb’, occultation statistics for < the100), period August in ‘dark(a limb’ (SZA ≥ 100).600 More details about the the solar il- data set that 2008 total of about 000 events, entire lumination condition and its consequences are given below. was available to us at the time of writing) are represented by histograms in Fig. 1. Of course, the lower number of 3occultations Retrieval method for the years 2002 and 2008 are caused by an incomplete sampling 3.1 Spectral behaviour of these years, while the smaller number in 2005 resulted from the instrument failure mentioned As alreadyLongitudinal said above, thesampling particle optical extinction specearlier. is clearly very homogeneous. trum is a priori unknown. Therefore, the actual optical specMost occultations occur at midlatitudes, although plenty of trum is treated as a product of the retrieval algorithm. It is polar are available. Mostshould starsbehave moderfar frommeasurements clear how such a particle optical spectrum parameterized, we can be and guided the factcold. that usual ate to weak but brightness, arebyrather Also, about half atmospheric particle sizeoccur distributions broad, covering a atmosphere of the occultations in theareSun-illuminated few orders of magnitude, and the resulting optical spectra are (“bright limb”, Zenith SZA<100), thus smooth. HenceSolar they are often Angle described with analytic,the other half in ‘dark limb’ such (SZA≥100). More about smooth functions, as polynomials. Fordetails data version 6.0,the solar illuthe GOMOScondition Science team to implement a quadratic mination andchose its consequences are given below. polynomial as a function of wavelength for the simple reason that it is versatile: large (constant spectrum), medium-sized (peak at mid-visible wavelengths) or small particle spectra 3 Rayleigh Retrieval method (the limit: extinction β depends on wavelength λ as β ∼ λ−4 ) can within good approximation be captured by polynomials. Retrieval algorithms for other satellite 3.1suchSpectral behaviour As already said above, the particle optical extinction spectrum is a priori unknown. Therefore, the actual optical spectrum is treated as a product of the retrieval algorithm. It is far from clear how such a particle optical spectrum should be parameterized, but we can be guided by the fact that usual atmospheric particle size distributions are broad, covering a few orders of magnitude, and the resulting optical spectra are thus smooth. Hence they are often described with analytic, smooth functions, such as polynomials. For data version 6.0, the GOMOS Science team chose to implement a quadratic Atmos. Chem. Phys., 10, 7997–8009, 2010 8000 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations polynomial as a function of wavelength for the simple reason that it is versatile: large (constant spectrum), medium-sized (peak at mid-visible wavelengths) or small particle spectra (the Rayleigh limit: extinction β depends on wavelength λ as β∼λ−4 ) can within good approximation be captured by such polynomials. Retrieval algorithms for other satellite occultation instruments are often also equipped with this feature. Furthermore, Vanhellemont et al. (2006) showed with simulated data (using a Mie code) that a quadratic polynomial is a good choice when one wants to obtain good aerosol retrievals without introducing too many degrees of freedom in the retrieval problem. other wavelengths (evaluated with the quadratic polynomial within the spectrometer A range 248-690 nm) are often very noisy. Finally, it should be mentioned that during the spectral inversion, the optical extinction spectra from the neutral air (Rayleigh scattering) are removed instead of retrieved from the measurements, using external ECMWF (European Centre for Medium-range Weather Forecasts) air density data, to avoid interferences with the residual scintillation and the spectrally similar aerosol contribution. Also, only spectrometer A measurements are currently used for the aerosol retrieval. 3.2 3.3 Spectral/spatial inversion The GOMOS retrieval algorithm has been described in detail in another paper of this special issue (Kyrölä et al., 2010). Here it suffices to say that the retrieval consists of two parts: (1) the spectral inversion, where measured transmittance spectra at each tangent altitude separately are inverted to slant path integrated column densities (for gases) and optical thickness (for particles), and (2) the spatial or vertical inversion, where the retrievals of the first step are separately inverted to local concentration profiles (gases) and optical extinction profiles (particles). This second step is performed in combination with a Tikhonov altitude smoothing (Twomey, 1985; Rodgers, 2000) in order to get partially rid of the perturbations caused by residual scintillation in measurements taken during very inclined occultations (Sofieva et al., 2009). The amount of smoothing is determined by a predetermined target resolution for the profile. For particles, a profile resolution of 4 km was chosen since unsmoothed profiles showed strong oscillations; aerosol extinction spectra have the tendency to swallow a large portion of the residual scintillation perturbations. Nevertheless, fine-scale structures (e.g. thin clouds) are smeared out due to this feature. The choice of 4 km for target resolution was based on the experience that it gave agreeable results; the actual magnitude of the residual scintillation perturbation on aerosol profiles is still not adequately determined, although it is known for the ozone retrievals (Sofieva et al., 2009). It is in the spectral inversion model that the slant path particle optical thickness is implemented as a quadratic polynomial: τ (λ)=σref (r0 + r1 1λ + r2 1λ2 ) with 1λ=λ − λref and λref =500 nm a reference wavelength. For scaling purposes, a “cross section” σref =6×10−10 cm2 was used. Notice that only the first parameter r0 has a direct physical meaning: σref r0 equals the particle slant path optical thickness at 500 nm. During the spatial inversion, this parameter receives Tikhonov-style altitude smoothing, while the other parameters remain unconstrained. Retrospectively, this turned out to be a poor methodology: while the obtained extinction profiles at 500 nm look quite good, the spectra at Atmos. Chem. Phys., 10, 7997–8009, 2010 The homogeneous layer assumption Occultation measurements have a limited information content. Hence the assumption of homogeneous atmospheric layers that is so often found in retrieval codes: the number of unknowns is drastically reduced, leading to a more stable inversion. For more or less uniformly mixed gases and particles (such as stratospheric aerosols), the assumption should hold quite well. However, when local phenomena (such as clouds) are observed, the assumption is wrong: the phenomenon affects the light ray only locally. This should be taken into account whenever we analyse retrievals of PSCs and volcanic plumes, for example: the obtained extinction coefficients should be seen as slant path equivalent values. 3.4 Bright limb versus dark limb retrievals When the optical light path traverses the Sun-illuminated atmosphere, parts of the atmosphere located in the fieldof-view scatter additional light into the instrument, which means that the simple optical transmission model for the retrieval is not correct anymore. This was anticipated: the additionnal upper and lower CCD bands in GOMOS were implemented to correct for this background illumination (Bertaux et al., 2010; Kyrölä et al., 2010). However, post-launch processing showed that the correction is not perfect. The situation is particularly bad for the aerosol extinction profiles, since their smooth optical extinction spectrum strongly resembles the limb signal. The aerosol extinction retrievals typically show unrealistic features at very high stratospheric altitudes. At present, the best we can do is exclude the bright limb profiles from data analysis. Investigations showed that occultation events with a solar zenith angle of 100◦ or larger deliver unperturbed, dark limb aerosol retrievals. 3.5 Retrieval results In summary, the GOMOS particle extinction profiles have acceptable quality around 500 nm, but are oversmoothed. At other wavelenghts, the profile quality is poor, and we therefore exclude them from further study. Furthermore, it is best to exclude the aerosol profiles in bright limb www.atmos-chem-phys.net/10/7997/2010/ Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations 40 30 Altitude [km] Altitude [km] 40 Polar stratospheric cloud 20 10 30 20 10 0 2 4 0 Extinction [km−1] −3 x 10 Background aerosol 40 30 20 10 2 4 Extinction [km−1] −3 x 10 Volcanic aerosol 40 Altitude [km] Altitude [km] Tropical subvisual cirrus 30 20 10 0 2 4 −1 −3 Extinction [km ] x 10 0 2 4 −1 −3 Extinction [km ] x 10 Fig. IndividualGOMOS GOMOS particle extinction profiles asFig. 2. 2. Individual particle extinction profiles withwith associsociated uncertainty: Polar Stratospheric Cloud (2003/7/30, ated uncertainty: a Polara Stratospheric Cloud (30/7/2003, 72,57◦ S, ◦ 72,57 S, 2.18 W), a subvisual tropical subvisual cirrus cloud (2002/10/7, 2.18◦◦W), a tropical cirrus cloud (7/10/2002, 0.52◦ S, ◦ ◦ ◦ 78.69S, E), background stratospheric aerosols (12/9/2003, 43.34◦ S, 0.52 78.69 E), background stratospheric aerosols (2003/9/12, ◦ ◦ ◦ 137.36S, W), volcanic stratospheric aerosols (9/1/2007, 4.52◦ S, 43.34 137.36 W), volcanic stratospheric aerosols (2007/1/9, ◦ ◦ E). All◦ plots have the same scale, in order to facilitate com27.15 4.52 S, 27.15 E). All plots have the same scale, in order to faciliparisons of magnitude. tate comparisons of magnitude. (SZA<100): from the entire data set of 600 000 occultaintroduce bias in the extinction profiles, as comparisons with tions, about 301 000 remain to be exploited. Among these, other instruments show (see below). some are still perturbed by residual scintillation. These perLike all are profiles derived from occultation measurements, turbations visible in individual aerosol extinction profiles. GOMOS aerosol extinction profiles are increasingly more When averaging large numbers of profiles (see e.g. the zonal uncertain when we descend to lower altitudes, because the plots below), the resulting mean profile becomes smooth. transmitted light intensity becomes weaker due to increasThere is reason to assume that the scintillation perturbations ing atmospheric gases, aerosols clouds. do not introduce extinction bias in the by extinction profiles, and as comparIn principle, a cut-off altitude can be defined, below which isons with other instruments show (see below). no Like aerosol information is present anymore. This altitude deall profiles derived from occultation measurements, pends on the wavelength considered, the magnitude and GOMOS aerosol extinction profiles and are increasingly more temperature of the and therefore changes from one the ocuncertain when westar, descend to lower altitudes, because transmitted light intensity becomes weaker due to increascultation to the next. At 500 nm, an average limit of 10 km ing be atmospheric gases, below aerosols and the clouds. can consideredextinction as a roughbyestimate which proIn principle, a cut-off altitude can be defined, below which files are not trustworthy anymore. noOn aerosol is present anymore. Thisextinction altitude deFig. information 2, we present individual GOMOS repends on the wavelength considered, and the magnitude and trievals at 500 nm for a number of particle types. It is impostemperature of the star, therefore one ocsible to distinguish theseand types using changes only onefrom wavelength; cultation to the next. At 500 nm, an average limit of 10 km the presented profiles were selected after analysis of the encan be considered as a rough estimate below which the protire GOMOS data set and knowledge about geolocation and files of areoccurence not trustworthy anymore. time of these particle phenomena (see further on in this paper). It is clear that the profiles are oversmoothed. For instance, www.atmos-chem-phys.net/10/7997/2010/ 8001 5 tropical subvisual clouds are known to be horizontally exOn Fig. 2, we present individual GOMOS extinction retended cloud layers that are quite thin, having a thickness trievals at 500 nm for a number of particle types. It is impossmaller than 1 km (Jensen et al., 1996); the example on the sible to distinguish these types using only one wavelength; figure clearlyprofiles shows that layer has spread the presented werethe selected afterbeen analysis of out the by en-the smoothing constraint. tire GOMOS data set and knowledge about geolocation and should mention here that phenomena the obtained(see particle timeWe of occurence of these particle furtherextinction retrievals sometimes assume negative values, usuon in this paper). ally at altitudes where the measured signals are low (below It is clear that the profiles are oversmoothed. For instance, the above-mentioned cut-off altitude), or horizontally where the particle tropical subvisual clouds are known to be exabundance is low (upper stratosphere and higher). This is tended cloud layers that are quite thin, having a thickness a logical consequence of ettheal.,fact that the the example last retrieval step 1996); on the smaller than 1 km (Jensen (spatial inversion) is linear and that the retrievals are not configure clearly shows that the layer has been spread out by the strained toconstraint. be positive. All further results that are discussed smoothing inWe thisshould paper mention were obtained by the processing data that here that obtainedofparticle ex-include negative values; discarding these wouldvalues, lead to usubiased tinction retrievals sometimes assume negative results. ally at altitudes where the measured signals are low (below the Quantifying above-mentioned cut-off extinction altitude), orretrieval where the particle the aerosol error is chalabundance low (upper stratosphere andfound higher). This ispalenging. Aisdetailed description can be in another aper logical consequence of the fact that the last retrieval of this GOMOS special issue (Tamminen et al., step 2010). (spatial inversion) is linear and that the retrievals are not conWe repeat the most important ideas and findings here. The strained be positive. All is further resultsby thattwo arecontributions discussed randomtoerror on a profile determined inthat thiswepaper were obtained by the processing of datanoise that which inmentioned before: (1) measurement clude negative discarding would due leadtotostar biased changes fromvalues; one stellar sourcethese to another magresults. nitude and temperature differences, and (2) the uncorrected Quantifying the aerosol extinctionAtretrieval is chal-the residual scintillation component. the timeerror of writing lenging. A detailed description can be found in another paGOMOS error estimation for the operational data products et al., 2010). per of this GOMOS special issue (Tamminen does not yet take the latter into account, so that retrieval erWe the most important ideas andinfluence findings of here. rorsrepeat are likely underestimated. The starThe magrandom error on a profile is determined by two contributions nitude is clear: brighter stars deliver a better signal-to-noise that we mentioned before:determines (1) the measurement which ratio. Star temperature the main noise spectral emischanges from one stellar source to another due to star magsion range: hot stars emit in the UV, colder ones in the visnitude and temperature differences, and (2) the uncorrected ible and near-infrared domain. The influence of star temresidual scintillation component. At the time of writing the perature on aerosol retrievals nevertheless remains limited; GOMOS error estimation for the operational data products it is star magnitude that plays the crucial role (Tamminen does not yet take the latter into account, so that retrieval eret al., 2010). Sources of systematic error are of course (1) rors are likely underestimated. The influence of star maga possibly wrong aerosol spectral model, and (2) an impernitude is clear: brighter stars deliver a better signal-to-noise fect ECMWF air density profile, the bothmain of which have been ratio. Star temperature determines spectral emisestimated by Tamminen et al. (2010). Retrieval errors are sion range: hot stars emit in the UV, colder ones in the vis- of course by standard propagation ible and calculated near-infrared domain. error The influence of through star tem-the retrievalon chain. Aerosol extinction error estimates bright perature aerosol retrievals nevertheless remains (for limited; of magnitude 30 % are obtained around an altitude 10 km, 2-10 itstars) is star that plays the crucial roleof(Tamminen from 15 toSources 25 km, and 10-50 % from km. (1) et%al., 2010). of systematic error25 aretoof40course As mentioned before,spectral the amount Tikhonov altitude a possibly wrong aerosol model,ofand (2) an impersmoothing is air determined by a predefined target resolution fect ECMWF density profile, both of which have been of 4 km, at by allTamminen altitudes, et regardless of Retrieval the star magnitude estimated al. (2010). errors are ofand temperature. Presentation averaging kernels is therefore course calculated by standardoferror propagation through the unnecessary; profile resolution is chosen in advance. retrieval chain. the Aerosol extinction error estimates (for bright stars) of 30% are obtained around an altitude of 10 km, 2– 10% from 15 to 25 km, and 10-50% from 25 to 40 km. 4 AsComparisons with other instruments mentioned before, the amount of Tikhonov altitude smoothing is determined by a predefined target resolution of detailed study for the GOMOS aerosol extinc4A km, at all validation altitudes, regardless of the star magnitude and tion profiles Presentation has not been of performed Nevertheless, Vantemperature. averagingyet. kernels is therefore hellemont etthe al. profile (2008)resolution already performed comparisons unnecessary; is chosen in advance. with the results derived from the imagers of the Atmospheric Atmos. Chem. Phys., 10, 7997–8009, 2010 Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations 7 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations GOMOS/SAGE II GOMOS/SAGE III 40 35 35 30 30 30 25 25 25 20 15 20 15 20 15 10 10 10 5 5 5 0 −200 −100 0 100 Relative difference [%] 200 0 −200 −100 0 100 Relative difference [%] GOMOS/POAM III 40 35 Altitude [km] Altitude [km] 40 Altitude [km] 8002 200 0 −200 −100 0 100 Relative difference [%] 200 Fig. 3. Comparison of GOMOS aerosol extinction profiles with other satellite measurements: SAGE II at 525 nm (left panel), SAGE III at 596 nm (middle panel) and POAM III at 603 nm (right panel). Shown are the statistics for the relative differences, calculated as Fig. 3. Comparison of GOMOS aerosol extinction profiles with other satellite measurements: SAGE II at 525 nm (left panel), SAGE 100 × 2(pGOMOS − pSAT )/|pGOMOS + pSAT |. The median of the set of relative differences is shown with full lines and dots. Dashed lines III at 596 nm (middleindicate panel) III16thatand 603 (right panel). Shown are the statistics for the relative differences, calculated as the and spread,POAM given by the 84thnm percentile. 100 × 2(pGOMOS − pSAT )/|pGOMOS + pSAT |. The median of the set of relative differences is shown with full lines and dots. Dashed lines indicate the spread, given by the 16th and 84th percentile. 40 Comparisons with other instruments 30 Alt. [km] 4 2002 40 30 2003 40 2004 40 2005 For the i-th coincidence, the difference between GOMOS 30 30 (GOM) and the other instrument (SAT), relative to the mean 20 of20the two, was evaluated as follows: Alt. [km] 20 A detailed validation study20 for the GOMOS aerosol extinction profiles has not been performed yet. Nevertheless, Van10 10 10 10 hellemont et al. (2008) already performed comparisons with (pGOM,i − pSAT,i ) −50 0 50 −50 0 50 −50 × 2 0 50 −50 0 50 1 =100 i the results derived from the imagers of the Atmospheric |pGOM,i + pSAT,i | x 10−3 2008 2006 2007 Chemistry Experiment ACE Here, 40 40 (Bernath et al., 2005). 40 1 we present first comparisons with aerosol extinction proAs statistical estimators for the entire data set, we prefered 30 30 30 0.8 files from the Stratospheric Aerosol and Gas Experiment to use the median (50th percentile) since it is more robust 0.6 20 20 II (SAGE II; see Chu et 20al. (1989)), its follow-up SAGE with respect to outliers than the numerical mean. The vari0.4 III (Thomason and Taha, 102003) and the Polar Ozone and ance of the data set was calculated 0.2 with the 16th and 84th 10 10 Aerosol Measurement POAM III (Lucke et al., 1999). As al0 estimates are shown in percentile. The50 obtained statistical −50 0 50 −50 0 50 −50 0 ready stated, only dark limb measurements were considered. Lat. [deg.] Lat. [deg.] Lat. [deg.] Fig. 3. As can be seen, the comparisons are quite good at Furthermore we avoided PSCs by excluding occultations inupper tropospheric/lower stratospheric altitudes. Differences side the polar vortex: apart thevalues wrong assumption of at 500 Fig. 4. Yearly from zonal median of (dark limb) aerosol extinction nm for the entireIIGOMOS mission. 20% All features that 10 are toto be 25 km, a conclusion with SAGE are within from present: theinstruments stratospheric aerosol layer,two PSCsdifin the Antarctic region, tropical subvisual cirrus clouds. Notice the enhanced homogeneous layers,expected two are different with that can2006. also bethatdrawn for the SAGE III comparisons. The stratospheric aerosol layer in 2007, resulting from the Soufrière Hills eruption in May Years are sampled incompletely: 2002 (start ferent viewing geometries will deliver two(instrument different profiles of the data set: August 2002), 2005 failure) and 2008 (end of available datadifferences set). median with POAM III are even smaller, within for the same cloud. This is less of a problem for tropical 10% from 11 to 22 km. Notice however that the variance is subvisual cirrus since they typically have a very wide hormuch larger than for the SAGE II/III comparisons. izontal extent and are very thin. A coincidence window of +/−250 km and +/−6 h was used, allowing us to find a fairly large comparison data set, summarized in Table 1. The ge5 Results ographic location of the obtained coincidences is mainly determined by the coverage of the used instruments (SAGE II, 5.1 Yearly zonal statistics SAGE III and POAM III) since GOMOS has a near-global coverage with several occultation latitudes per orbit. Notice A coarse idea about the presence of aerosols and clouds in that we used a spectral channel of each instrument that is the upper troposphere/lower stratosphere can be gained by close to the GOMOS reference wavelength of 500 nm. Furconsidering zonal yearly statistics. Ranging from 90◦ S to thermore, GOMOS data were interpolated to these wave90◦ N, 72 latitude bins with a width of 2.5 degrees were delengths using the retrieved quadratic polynomial. We should fined. Aerosol extinction profiles were linearly interpolated also mention that no effort was made to match the vertical on a common altitude grid ranging from 1 to 50 km with a resolution between two instruments with averaging kernels; spacing of 1 km. Yearly statistics were subsequently calcuthis will certainly be done in a full validation study in the lated on all data within one bin. Once again: we used perfuture. centiles as statistical estimators since extinction values are not necessarily normally distributed and because the median (50th percentile) is rather insensitive to outliers. We should Atmos. Chem. Phys., 10, 7997–8009, 2010 www.atmos-chem-phys.net/10/7997/2010/ 15 15 15 10 10 10 5 5 5 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations 0 −200 −100 0 100 Relative difference [%] 200 0 −200 −100 0 100 Relative difference [%] 0 −200 200 8003 −100 0 100 Relative difference [%] 200 Table 1. GOMOS aerosol extinction retrievals: comparison data set; coincidence window: (500 km, 1/2 day) Fig. 3. Comparison of GOMOS aerosol extinction profiles with other satellite measurements: SAGE II at 525 nm (left panel), SAGE Instrument Version Wavelength # of coincidences Time period considered III at 596 nm (middle panel) and POAM III at 603 nm (right panel). Shown are the statistics for the relative differences, calculated as 100 × 2(pGOMOS − pII SAT )/|pGOMOS + pSAT |. The median of the set of relative differences is shown with full lines and dots. Dashed lines SAGE 6.20 525 nm 6227 27 August 2002–March 5, 2005 indicate the spread, given by the 16th and 84th percentile. SAGE III POAM III 2002 40 Alt. [km] 3.00 4.00 596 nm 603 nm 6258 11 641 2003 40 7 November 2002–3 December 2005 26 August 2002–3 December 2005 2004 40 30 30 30 30 20 20 20 20 10 10 10 10 −50 0 50 2006 40 −50 0 50 2007 40 −50 0 50 −50 0 50 −3 2008 40 2005 40 x 10 Alt. [km] 1 30 30 30 20 20 20 10 10 10 −50 0 50 Lat. [deg.] −50 0 50 Lat. [deg.] 0.8 0.6 0.4 0.2 −50 0 50 Lat. [deg.] 0 Fig. 4. Yearly zonal median values of (dark limb) aerosol extinction at 500 nm for the entire GOMOS mission. All features that are to be Fig. 4. Yearly zonal median values of (dark limb) aerosol extinction at 500 nm for the entire GOMOS mission. All features that are to be expected are present: the stratospheric aerosol layer, PSCs in the Antarctic region, tropical subvisual cirrus clouds. Notice the enhanced expectedstratospheric are present: the stratospheric aerosolfrom layer, PSCs inHills theeruption Antarctic region, clouds.2002 Notice aerosol layer in 2007, resulting the Soufrière in May 2006. tropical Years thatsubvisual are sampledcirrus incompletely: (start the enhanced stratospheric in2002), 2007,2005 resulting fromfailure) the Soufrière eruption May of theaerosol data set:layer August (instrument and 2008Hills (end of availablein data set).2006. Years that are sampled incompletely: 2002 (start of the data set: August 2002), 2005 (instrument failure) and 2008 (end of available data set). also mention that yearly zonal statistics are seasonally biased when we use only dark limb measurements, since Arctic/Antarctic summer is not sampled. The median particle extinction at 500 nm is shown in Fig. 4 for every GOMOS mission year. A few phenomena are readily observed: (1) the umbrella-shaped stratospheric aerosol layer that is highest at the equator, lowest at the poles, (2) higher extinction values in the Antarctic (and to a lesser extent Arctic) stratosphere that are caused by PSCs, and (3) higher extinction values in a localized tropical zone at an altitude of about 16– 17 km due to subvisual cirrus clouds. The picture is almost systematic for every year, but there are some significant differences however. First notice that Antarctic PSCs are less pronounced for the years 2002 and 2008 because the Antarctic PSC season is not well sampled in those years: the data set starts end of August 2002 and ends in May 2008. More important, stratospheric aerosol extinction levels are much higher in 2007 and remain elevated even in 2008, suggesting the formation of new aerosols following stratospheric injection of SO2 by a volcanic eruption. This is the case; the Soufrière Hills eruption (see below) in May 2006 is most www.atmos-chem-phys.net/10/7997/2010/ likely the source. Furthermore, 2005 also seems to exhibit elevated aerosol levels, although the picture is noisier due to the incomplete sampling of the year (instrument failure). Equally interesting is the yearly zonal variability of the 500 nm aerosol extinction values, calculated as half the difference between the 84th and 16th percentile. The variability is of course determined by the S/N-ratio of the measurements and (more importantly) by natural aerosol/cloud variability, caused by the appearing, disappearing and atmospheric transport of particles. This is clearly visible on Fig. 5. Typical “on/off-events” such as clouds (tropical cirrus, PSCs) exhibit large variability, while slowly changing features (such as the stratospheric aerosol layer) vary little within one year. Notice once again that the Antarctic PSC variability during 2002 and 2008 is weak since these years have not been completely sampled. At lower, tropospheric altitudes, we see large variability due to a combination of larger profile uncertainty (measured signals are weaker) and tropospheric clouds. Atmos. Chem. Phys., 10, 7997–8009, 2010 8004 Version Wavelength # of coincidences Time period considered SAGE II SAGE III POAM III 6.20 3.00 4.00 525 nm 596 nm 603 nm 6227 6258 11641 August 27, 2002 - March 5, 2005 November 7, 2002 - December 3, 2005 August 26, 2002 - December 3, 2005 2002 40 Alt. [km] Instrument F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations 2003 40 2004 40 30 30 30 30 20 20 20 20 10 10 10 10 −50 0 50 −50 2006 40 0 50 2007 40 −50 0 2005 40 50 −50 0 −3 2008 40 50 x 10 Alt. [km] 1 30 30 30 20 20 20 10 10 10 −50 0 50 Lat. [deg.] −50 0 50 Lat. [deg.] 0.8 0.6 0.4 0.2 −50 0 0 50 Lat. [deg.] Fig. 5. Yearly zonal variability of (dark limb) aerosol extinction at 500 nm for the entire GOMOS mission. Variability is calculated as half Fig. 5. Yearly zonal variability of (dark limb) aerosol extinction at 500 nm for the entire GOMOS mission. Variability is calculated as the difference of the 84th and 16th percentile, and is determined by measurement error and (more importantly) by natural aerosol/cloud half the difference of the 84thevents and 16th percentile, and cirrus, is determined by measurement (morewhile importantly) by natural variability. ’On/off’ such as clouds (tropical Antarctic PSCs) of course exhibiterror large and variability, slowly changing features aerosol/cloud (backgrounds aerosol vary little. Years that are sampled incompletely: (start of the large data set: august 2002), 2005slowly (instrument variability. “On/off” events suchlayer) as clouds (tropical cirrus, Antarctic PSCs) of 2002 course exhibit variability, while changing features andlayer) 2008 (end of available data set). (backgroundsfailure) aerosol vary little. Years that are sampled incompletely: 2002 (start of the data set: august 2002), 2005 (instrument failure) and 2008 (endVanhellemont of available data set). Aerosol/Cloud Extinction observations et al.: GOMOS 9 Aerosol. Ext. [1/km] uary 27 and 28 (Kamei et al., 2006). Manam is one of 2006, in a tropical latitude band from 6◦ N to 26◦ N. Three the most active volcanoes in the region; the above mendistinct periods can −3 be seen. First, we observe low back° ° 2004 to 2006 − Aerosol ext. 500 nm, alt. = 20 km, lat. = 6 N − 26 N x 10 tioned eruptions followed ongoing volcanic activity that ground aerosol 3levels until the end of 2004. Second, from started already in October 2004. An image taken by the early 2005 to the beginning of June 2006, large data gaps infrared Aqua/MODIS (Moderate Resolution Imaging Specare present due2.5to instrument failure. Nevertheless, the data troradiometer) indicates that the ash clouds of the first erupseem to suggest a declining tail following a volcanic erup2 we take the small set of data points at early tion on Jan. 27 reached to over 20 km altitude, well into tion, especially if the stratosphere. The ash clouds of the second eruption on 2005 into account. And third, in early July 2006 we observe 1.5 by about a factor of 3 in extinction levels. Jan. 28 ascended to 18 km altitude (Smithsonian Institution, a sudden increase 2005). Several days later, stratospheric aerosol layers were The same conclusions are drawn when inspecting the evolu1 detected twice between about 18 to 20 km altitude (layer tion in latitude and time on Fig. 7. It is clear that at least two thickness ranging from 0.2 to 1.4 km) by a shipboard lidar usvolcanic events in the tropics should be considered. 0.5 ing a Nd:YAG laser operated at 1064 nm and 532 nm (Kamei The elevated values in 2005 are most likely caused by et al., 2006). The layers were detected in the Western Pacific stratospheric sulfate aerosols, formed out of the SO2 cloud 0 around 0 - 2◦ N, 156◦ E (Feb. 3-4 2005) and 7 - 9◦ N, 156◦ E injected in the stratosphere by the eruptions of the Manam ◦ ◦ (Feb. 9 - 10). Inspecting Fig. 7, we see that the amount of volcano (Papua New Guinea, 4.080 S, 145.037 E) on Jan−0.5 −1 Feb04 Jun04 Sep04 Dec04 Mar05 Jul05 Date Oct05 Jan06 May06 Aug06 Nov06 Fig. 6. A 2004-2006 GOMOS aerosol extinction time series at an altitude of 20 km. All data within a latitude band from 6◦ N - 26◦ N are Fig. 6. A 2004-2006shown. GOMOS extinction an altitude 20 km. data within a latitude band from 6–26◦ N are Clearly aerosol visible are the background time aerosol series conditionat in 2004, the possibleof declining tail ofAll the post-eruptive aerosols resulting from Manam (Papua New Guinea, condition Jan. 27-28, 2005; first vertical and thedeclining enhanced aerosol following the eruption aerosols of shown. Clearly visibletheare the volcano background aerosol in 2004, the line), possible tail levels of the post-eruptive resulting from Soufrière Hills (Montserrat, May 20, 2006, second vertical line). the Manam volcano (Papua New Guinea, Jan. 27-28, 2005; first vertical line), and the enhanced aerosol levels following the eruption of Soufrière Hills (Montserrat, 20 May 2006, second vertical line). injected sulfur was large enough to leave a significant aerosol trace in the GOMOS data during the largest part of 2005. The source for the elevated aerosol levels in the second 5.2 Volcanic stratospheric aerosols half of 2006 and 2007 has been identified as the eruption of the Soufrière Hills volcano (16.72◦N, 62.18◦W, Montserrat, West Indies), on May 20, 2006. Immediately following the collapse of the eastern volcano flank, an eruption column The observed elevated extinction levels in 2005 reof ash and gases rose to at least 17 km. and Prata2007 et al. (2007) usedinvestigation. a combination of satellite instruments quire a more detailed On Fig. 6, we(Aqua/AIRS, present MSG/SEVIRI, MLS, OMI and CALIPSO/CALIOP) to reaerosol extinction values altitude of 20 km (which constructat thean event and its immediate aftermath. Theylies found an estimated 0.1 Tg(S)for was injected in the stratosphere above the subvisualthatcirrus altitudes) the period 2004– in the form of SO2 , after which the gas cloud west◦ traveled 2006, in a tropical latitude 6◦20Nkm. to 26 Three ward at an band altitudefrom of about CarnN. et al. (2007) on the other hand used OMI data to obtain an estimated 0.22 Tg of SO2 . They also reported CALIPSO/CALIOP lidar 10, backscatter measurements of the associated stratospheric Atmos. Chem. Phys., 7997–8009, 2010 aerosol layer as early as June 7, 2006, at an altitude of 20 km. The layer remained visible in the CALIOP data until July 6. However, as Thomason et al. (2007) remarked, in general the stratospheric aerosol layer remains quite invisible in CALIOP backscatter measurements, while occulation instru- path lengths. Nevertheless, very recently Vernier et al. (2009) showed how CALIPSO/CALIOP backscatter data improved strongly after the introduction of a new cloud mask and a new calibration, and howcan an improved stratospheric distinct periods be seen. First,aerosol we observe low backpicture emerged after sufficient data averaging. In any case, ground aerosol levels until the end of 2004. Second, from the fact that GOMOS identifies stratospheric sulfate aerosols early to the June 2006, large data gaps well after2005 the eruption datebeginning is illustrated inof Fig. 8, which shows the appearing and poleward transport of the sulfuric are present due to instrument failure. Nevertheless, the data acid particles. seem a declining tail following a volcanic erupFigs. 7to andsuggest 8 also indicate that it took roughly one year for the Soufrière Hills aerosol the entireset globe. tion, especially if wecloud taketo cover the small of data points at early Elevated extinction levels remained present until at least the 2005 into Inaccount. third, earlyHills July 2006 we observe end of 2007. the monthsAnd following the in Soufrière eruption, a few other eruptions possibly impacted the stratospheric aerosol layer. Hofmann et al. (2009) briefly mentioned the July 14, 2006 Tungurahua eruption (Ecuador, 1,467◦S, 78,442◦W), less www.atmos-chem-phys.net/10/7997/2010/ than a month after the Soufrière Hills eruption. And Thomason et al. (2007) showed CALIOP observations of the volcanic plume resulting from the October 7, 2006 Tavurvur eruption (Rabaul, Papua New Guinea, 4.271◦S, 152.203◦E). Both are equatorial volcanoes that possible injected sulfur into the stratosphere, hereby enhanc- 10 Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations Lat. [deg.] x 10 2 45 1.5 0 1 −45 −90 Jan05 0.5 Jan06 Jan07 Jan08 x 10 2 45 1.5 0 1 −45 −90 Jan05 0 −3 Aerosol extinction (500 nm) at 20 km altitude 90 Lat. [deg.] −3 Aerosol extinction (500 nm) at 18 km altitude 90 8005 0.5 Jan06 Jan07 Jan08 0 Fig. 7. Checkerboard plots showing the median of binned 500 nm aerosol extinction data as function of latitude and time, at an altitude 7. Checkerboard showing the panel). median ofNotice binned 500 aerosol extinction data early as function of latitude and the time,end at anofaltitude 18 The global of 18 km Fig. (upper panel) andplots 20 km (lower thenm elevated values after 2005, and after May of 2006. and in 20 the km (lower panel). Notice the elevated values after early 2005, and after the end of May 2006. The global spreading spreadingkm is (upper clearlypanel) visible latter case. is clearly visible in the latter case. a suddenetincrease by From aboutGOMOS a factordata of 3it in levels. al. (2009). is extinction at present unclear or not the are existing volcanic layer was The samewether conclusions drawn whenaerosol inspecting thereplenevoluished with sulfate aerosols fromat these eruption in latitude andnew time on Fig. 7. Itoriginating is clear that least two volcanictions. events in the tropics should be considered. The elevated values in 2005Clouds are most likely caused by 5.3 Polar Stratospheric stratospheric sulfate aerosols, formed out of the SO2 cloud detects PSCs quite well. Strongly of enhanced optiinjected GOMOS in the stratosphere by the eruptions the Manam extinction measured4.080 every◦year in the Antarctic ◦ E) onPSC volcano cal (Papua NewisGuinea, S, 145.037 Janseason (roughly from the end of May to October), with valuary 27 ues andtypically 28 (Kamei et al., 2006). Manam is one of 3 or 4 times larger than in normal background the mostconditions. active volcanoes in the region; the above menThese kind of criteria (latitude, time of year, extioned eruptions followed ongoing volcanic activity that tinction values above a certain treshold) allow us to identify the presence of a PSC. 2004. It is however that by is the started already in October An temperature image taken the driver for the formation Resolution of PSCs, as can be seen on infrared main Aqua/MODIS (Moderate Imaging Specthe top panel of Fig. 9. Shown are all GOMOS aerosol extroradiometer) indicates that the ash clouds of the first eruptinction measurements at 500 nm taken in 2004 at an alti◦ tion on 27 January to over 20from km 90 altitude, into tude of 20 kmreached for the latitude band S to 55◦well S. Temthe stratosphere. The ash cloudsfrom of the second product eruption perature data were obtained the GOMOS fileson consist oftoECMWF The selected data Jan. 28and ascended 18 kmanalysis altitudeprofiles. (Smithsonian Instituset represents of measurements insideaerosol and outside tion, 2005). Severala mixture days later, stratospheric laythe Antarctic vortex (PSCs and stratospheric aerosols), but ers wereplotted detected twice between about 18 to 20 km altitude against temperature the differentiation is very clear: (layer thickness to195 1.4 K, km) a shipboard clouds areranging formed from below 0.2 about theby known formalidar using Nd:YAG laser operated 1064Itnm and 532less nm tionatemperature of NAT and STSatPSCs. is however clear the data not Type II PSCs at even al.,from 2006). Thewhether layers or were detected in form the Western (Kamei et ◦ E (3–4 lower temperatures. Ideally, differentiation of 2005) differentand types7– Pacific around 0–2◦ N, 156 February ◦ ◦ 9 N, 156 E (9–10 February). Inspecting Fig. 7, we see that the amount of injected sulfur was large enough to leave a significant aerosol trace in the GOMOS data during the largest part of 2005. The source for the elevated aerosol levels in the second half of 2006 and 2007 has been identified as the eruption of the Soufrière Hills volcano (16.72◦ N, 62.18◦ W, Montserrat, West Indies), on 20 May 2006. Immediately following the collapse of the eastern volcano flank, an eruption column www.atmos-chem-phys.net/10/7997/2010/ Prata et al. (2007) of ash gases rose at least 17 km. of PSC withand UV/Vis/NIR datato should be done by inspecting particle of theinstruments associated opti-(Aqua/AIRS, usedsize a distributions, combinationor the of shape satellite calMSG/SEVIRI, spectrum. MethodsMLS, have already in the past OMI been and devised CALIPSO/CALIOP) to refor the SAGE and POAM instruments to make a distinction construct the event and its immediate aftermath. They found between Type Ia and Ib particles, based on the assumption estimated 0.1than Tg(S) was injected in the stratosphere thatthat the an latter are smaller the former, with a different in the form of SO , after which the gas cloud traveled westextinction spectrum as a2 consequence (Strawa et al., 2002; Poole et al., The second panel of20Fig. ward at 2003). an altitude of about km.9 shows Carntheet al. (2007) ratio 600 other nm to 400 nm used GOMOS optical extinction. The-an estimated onofthe hand OMI data to obtain oretically, very small particles (β(λ) ∼ λ−4 ) should lead to a 0.22 Tg of SO2 . They also reported CALIPSO/CALIOP livalue of 0.2, while large particles (β(λ) = constant) should dara value backscatter measurements of the associated have of 1. The data are extremely noisy due to thestratospheric aerosol layer as early as 7 June 2006, at iman altitude of already mentioned problem with the aerosol spectral law plementation. the data cloud in is more or less data until 20 km. TheNevertheless, layer remained visible the CALIOP situated between the theoretical limits,etand particles 6 July. However, as Thomason al.larger (2007) remarked, in genare observed below 195 K, as expected. The data show also eral the stratospheric aerosol layer remains quite invisible in that it is currently impossible to differentiate between differentCALIOP PSC types.backscatter measurements, while occulation instru- ments such as SAGE II have no problem with the detection. No doubt this is caused by the preferential forward scattering The presented PSC results do notinadd significantly with new inof light by small particles, combination longer optical formation to the current knowledge on PSC formation; for Vernier et al. (2009) path lengths. Nevertheless, very recently this, much more detailed analysis is needed (taking into acshowed how CALIPSO/CALIOP backscatter data count all thermodynamic parameters and air parcel dynam- improved strongly the measurements introduction clearly of a new cloud ics). But theafter GOMOS contain ele- mask and a ments particle new(temperature calibration,dependence and how of anextinction improvedandstratospheric aerosol sizes) that are crucial inafter such sufficient a detailed study. picture emerged data averaging. In any case, the fact that GOMOS identifies stratospheric sulfate aerosols well after the eruption date is illustrated in Fig. 8, which shows the appearing and poleward transport of the sulfuric acid particles. Figures 7 and 8 also indicate that it took roughly one year for the Soufrière Hills aerosol cloud to cover the entire globe. Elevated extinction levels remained present until at least the end of 2007. In the months following the Soufrière Hills eruption, a few other eruptions possibly impacted the Atmos. Chem. Phys., 10, 7997–8009, 2010 Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations 11 8006 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations May 2006 Alt. [km] 30 June 2006 30 July 2006 30 30 20 20 20 20 10 10 10 10 −3 x 10 2 Aug. 2006 1.8 1.6 −50 Alt. [km] 50 Sep. 2006 30 −50 0 50 Oct. 2006 30 20 10 −50 0 50 Jan. 2007 10 −50 0 50 Nov. 2006 30 20 30 Alt. [km] 0 0 50 Feb. 2007 30 10 0 50 1.2 20 −50 30 0 50 Lat. Mar. 2007 10 1 0.8 −50 30 0 50 Lat. Apr. 2007 20 20 20 0.2 15 10 −50 0 Lat. 50 10 −50 0 Lat. 50 10 −50 0 Lat. 50 10 0.6 0.4 25 20 1.4 Dec. 2006 30 20 −50 −50 −50 0 Lat. 50 0 8. Evolution volcanic stratospheric aerosolsresulting resultingfrom fromthe theSoufrière SoufrièreHills Hillseruption eruptionon onMay 20 May Fig.Fig. 8. Evolution of of thethe volcanic stratospheric aerosols 20, 2006. 2006. Shown Shown are are monthly monthly zonal median aerosol extinction coefficients at 500 nm. Starting from the eruption site (Montserrat, 16.72◦◦ N, 62.18◦◦ W), the plume disperses zonal median aerosol extinction coefficients at 500 nm. Starting from the eruption site (Montserrat, 16.72 N, 62.18 W), the plume disperses poleward and encircles the entire earth within a year. poleward and encircles the entire earth within a year. stratospheric aerosol layer. Hofmann et al. (2009) briefly 6 Conclusions mentioned the 14 July 2006 Tungurahua eruption (Ecuador, 1,467◦ S, 78,442◦ W), less than a month after the Soufrière The current GOMOS operational aerosol/cloud product conHills eruption. And Thomason et al. (2007) showed CALIOP sists of optical extinction profiles at 500 nm and additional observations of the volcanic plume resulting from the Octospectral to evaluate extinction at other waveber 7,coefficients 2006 Tavurvur eruptionthe (Rabaul, Papua New Guinea, lengths as well. The quality of the product is not optimal ◦ ◦ 4.271 S, 152.203 E). Both are equatorial volcanoesyet, that duepossible to a problematic spectral combined injected sulfur intolaw the implementation, stratosphere, hereby enhancwith altitude smoothing that is tooHills strong. Furthermore, inganthe already existing Soufrière perturbation. The profiles derived from bright limb measurements currently Tavurvur case was recently demonstrated inare a convincing notway usable. Nevertheless, we restrict ourselvesdata to the of using the improvedifCALIPSO/CALIOP by use Vernier 500etnm extinction profiles retrieved from dark limb measureal. (2009). From GOMOS data it is at present unclear ments, then can be considered as layer good,was although wether or the not quality the existing volcanic aerosol replenfineished structure (thin cirrus clouds, cloud inhomogeneities with new sulfate aerosols originating from these etc.) eruphastions. been smoothed. For the first time, a comparison with SAGE II, SAGE III and POAM III was presented, showing good within 20 % Clouds in the upper troposphere/lower 5.3agreement Polar Stratospheric stratosphere, from 10 km to about 25 km. All the atmospheric typesStrongly that areenhanced expectedoptito GOMOS detects PSCsparticle quite well. be cal observed by aissatellite occultation instrument have been extinction measured every year in the Antarctic PSC detected GOMOS: sulfate seasonby (roughly fromthe thebackground end of May stratospheric to October), with valaerosol layer (or layer) typical background umbrellaues typically 3 orJunge 4 times largerwith thanits in normal shaped form, sulfate aerosols from volcanic conditions. These kind of criteria (latitude, origin, time of tropical year, exsubvisual below the tropopause at identify an altinctioncirrus valuesclouds above ajust certain treshold) allow us to titude of about 16-17 km, and PSCs in the polar regions. Atmos. Chem. Phys., 10, 7997–8009, 2010 the presence of a PSC. It is however temperature that is the The cloud-type events (PSCs and cirrus) have a strong yearly main driver for the formation of PSCs, as can be seen on variability, while the Junge layer remains remarkably conthe top panel of Fig. 9. Shown are all GOMOS aerosol exstant within one year. tinction measurements at 500 nm taken in 2004 at an altiTheoflast SO2band injection into stratosphere ◦ Sthe ◦ S. Temtude 20 major km forvolcanic the latitude from 90 to 55 dates already from almost 18 years ago (Mount Pinatubo, perature data were obtained from the GOMOS product files 1991), with the consequence that current aerosol levels are and consist of ECMWF analysis profiles. The selected data extremely low. So low that the effect of ‘moderate’ volset represents a mixture of measurements inside and outside canic eruptionsvortex becomes in the GOMOS aerosol the Antarctic (PSCsvisible and stratospheric aerosols), but record. One might wonder if the so-called background is not plotted against temperature the differentiation is very clear: only maintained bybelow the typically mentioned sources (OCS, clouds are formed about 195 K, the known formation recently even anthropogenic sulfate from coal burning in temperature of NAT and STS PSCs. It is however less clear China), but as well by these moderate volcanic eruptions, that from the data whether or not Type II PSCs form at even are much weaker thanIdeally, the catastrophic events (Mt. Pinatubo, lower temperatures. differentiation of different types Mt. St. Helens, El Chichón), but much more frequent. Here, of PSC with UV/Vis/NIR data should be done by inspecting for the first time, the aerosol enhancements resulting from particle size distributions, or the shape of the associated optithe Manamhave (Papua Newbeen Guinea) andinSoufrière caleruptions spectrum.of Methods already devised the past for the SAGE and West POAM instruments to make a distinction Hills (Montserrat, Indies) have been identified in the between data. Type Ia Ib particles, based onwas the assumption GOMOS In and the latter case, GOMOS clearly able thethe latter aredispersion smaller than theaerosols. former, with different tothat track global of the In thea aftermath et al.,in2002; spectrum as a consequence (Strawa ofextinction the eruption, two other possible intrusions should prinPoolebeetvisible: al., 2003). The second panel and of Fig. 9 shows the ciple Tungurahua (Ecuador) Tavurvur (Papua ratio Guinea). of 600 nmWe to 400 nmtoGOMOS extinction. TheNew hope identifyoptical them in future aerosol oretically, very small particles (β(λ)∼λ−4 ) should lead to a profile improvements. The dynamics of PSCs have been studied previously with www.atmos-chem-phys.net/10/7997/2010/ F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations x 10 2 1.5 1 www.atmos-chem-phys.net/10/7997/2010/ Acknow cial aid the Eur (Contra GOMO 0.5 0 −0.5 −1 180 Conclusions The current GOMOS operational aerosol/cloud product consists of optical extinction profiles at 500 nm and additional spectral coefficients to evaluate the extinction at other wavelengths as well. The quality of the product is not optimal yet, due to a problematic spectral law implementation, combined with an altitude smoothing that is too strong. Furthermore, profiles derived from bright limb measurements are currently not usable. Nevertheless, if we restrict ourselves to the use of 500 nm extinction profiles retrieved from dark limb measurements, then the quality can be considered as good, although fine structure (thin cirrus clouds, cloud inhomogeneities etc.) has been smoothed. For the first time, a comparison with SAGE II, SAGE III and POAM III was presented, showing good agreement within 20% in the upper troposphere/lower stratosphere, from 10 km to about 25 km. All the atmospheric particle types that are expected to be observed by a satellite occultation instrument have been detected by GOMOS: the background stratospheric sulfate aerosol layer (or Junge layer) with its typical umbrellashaped form, sulfate aerosols from volcanic origin, tropical subvisual cirrus clouds just below the tropopause at an altitude of about 16–17 km, and PSCs in the polar regions. The cloud-type events (PSCs and cirrus) have a strong yearly variability, while the Junge layer remains remarkably constant within one year. The last major volcanic SO2 injection into the stratosphere dates already from almost 18 years ago (Mount Pinatubo, 1991), with the consequence that current aerosol levels are extremely low. So low that the effect of “moderate” volcanic eruptions becomes visible in the GOMOS aerosol record. One might wonder if the so-called background is not only maintained by the typically mentioned sources (OCS, recently even anthropogenic sulfate from coal burning in China), but as well by these moderate volcanic eruptions, that are much weaker than the catastrophic events (Mt. Pinatubo, Mt. St. Helens, El Chichón), but much more frequent. Here, 2004, alt. = 20 km, lat. = 90S − 55S 2.5 190 200 210 Temperature [K] 220 230 Refere 2004, alt. = 20 km, lat. = 90S − 55S 1 Aerosol Ext. ratio [no units] 6 −3 3 Aerosol Ext. [1/km] value of 0.2, while large particles (β(λ)=constant) should have a value of 1. The data are extremely noisy due to the already mentioned problem with the aerosol spectral law implementation. Nevertheless, the data cloud is more or less situated between the theoretical limits, and larger particles are observed below 195 K, as expected. The data show also that it is currently impossible to differentiate between different PSC types. The presented PSC results do not add significantly new information to the current knowledge on PSC formation; for this, much more detailed analysis is needed (taking into account all thermodynamic parameters and air parcel dynamics). But the GOMOS measurements clearly contain elements (temperature dependence of extinction and particle sizes) that are crucial in such a detailed study. 8007 0.8 0.6 0.4 0.2 0 180 GOMO PSC te that pa This is crophy As o projec improv aeroso the clo be dev bution cle phe 190 200 210 Temperature [K] 220 230 Fig. measurements of of Polar Polar Stratospheric Stratospheric Clouds. Clouds. Top Top Fig. 9. 9. GOMOS GOMOS measurements panel: at 500 500 nm nm versus versus temperature temperature at at an an altitude altitude panel: optical optical extinction extinction at of km, for for all all dark dark limb limb occultations occultations in in 2004 2004 at at latitudes latitudes below below of 20 20 km, 55◦◦ S. S. Bottom Bottom panel: panel: extinction extinction ratio ratio (600/400 (600/400 nm), 55 nm), derived derived from from the same same measurements. measurements. the for the first time, the aerosol enhancements resulting from the eruptions of Manam (Papua New Guinea) and Soufrière Hills (Montserrat, West Indies) have been identified in the GOMOS data. In the latter case, GOMOS was clearly able to track the global dispersion of the aerosols. In the aftermath of the eruption, two other possible intrusions should in principle be visible: Tungurahua (Ecuador) and Tavurvur (Papua New Guinea). We hope to identify them in future aerosol profile improvements. The dynamics of PSCs have been studied previously with GOMOS data (Vanhellemont et al., 2005). The dependence of PSC formation on temperature is a complex study topic. In this paper, we only showed a first qualitative analysis with GOMOS data, the results of which agree with the theoretical Atmos. Chem. Phys., 10, 7997–8009, 2010 Bernath ler, P.-F. Dufo Jenn Cone wint Roch R., S D., W der, Miss doi:1 Bertaux for a obse Bertaux R., K trend in Sp Bertaux F., S O., B Saav culta ENV Carn, S Krue serva sphe Chin, M a so Geop 8008 F. Vanhellemont et al.: GOMOS Aerosol/Cloud Extinction observations PSC temperature dependence. The data show also roughly that particle size information is present in the GOMOS data. This is an important conclusion for future studies on the microphysics of PSCs. 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