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    Aerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters
    (Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.
    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.
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    The potential of elastic and polarization lidars to retrieve extinction profiles
    (Katlenburg-Lindau : Copernicus, 2020) Giannakaki, Elina; Kokkalis, Panos; Marinou, Eleni; Bartsotas, Nikolaos S.; Amiridis, Vassilis; Ansmann, Albert; Komppula, Mika
    A new method, called ElEx (elastic extinction), is proposed for the estimation of extinction coefficient lidar profiles using only the information provided by the elastic and polarization channels of a lidar system. The method is applicable to lidar measurements both during daytime and nighttime under well-defined aerosol mixtures. ElEx uses the particle backscatter profiles at 532 nm and the vertically resolved particle linear depolarization ratio measurements at the same wavelength. The particle linear depolarization ratio and the lidar ratio values of pure aerosol types are also taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. In this study, ElEx was applied in an aerosol mixture of marine and dust particles at Finokalia station during the CHARADMExp campaign. Any difference between ElEx and Raman extinction profiles indicates that the nondust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun photometer aerosol optical depth observations is performed as well during daytime. Differences in the total aerosol optical depth are varying between 1.2 % and 72 %, and these differences are attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to the overlap problem. © 2020 Author(s).
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    EARLINET evaluation of the CATS Level 2 aerosol backscatter coefficient product
    (Katlenburg-Lindau : EGU, 2019) Proestakis, Emmanouil; Amiridis, Vassilis; Marinou, Eleni; Binietoglou, Ioannis; Ansmann, Albert; Wandinger, Ulla; Hofer, Julian; Yorks, John; Nowottnick, Edward; Makhmudov, Abduvosit; Papayannis, Alexandros; Pietruczuk, Aleksander; Gialitaki, Anna; Apituley, Arnoud; Szkop, Artur; Muñoz Porcar, Constantino; Bortoli, Daniele; Dionisi, Davide; Althausen, Dietrich; Mamali, Dimitra; Balis, Dimitris; Nicolae, Doina; Tetoni, Eleni; Liberti, Gian Luigi; Baars, Holger; Mattis, Ina; Stachlewska, Iwona Sylwia; Voudouri, Kalliopi Artemis; Mona, Lucia; Mylonaki, Maria; Perrone, Maria Rita; Costa, Maria João; Sicard, Michael; Papagiannopoulos, Nikolaos; Siomos, Nikolaos; Burlizzi, Pasquale; Pauly, Rebecca; Engelmann, Ronny; Abdullaev, Sabur; Pappalardo, Gelsomina
    We present the evaluation activity of the European Aerosol Research Lidar Network (EARLINET) for the quantitative assessment of the Level 2 aerosol backscatter coefficient product derived by the Cloud-Aerosol Transport System (CATS) aboard the International Space Station (ISS; Rodier et al., 2015). The study employs correlative CATS and EARLINET backscatter measurements within a 50km distance between the ground station and the ISS overpass and as close in time as possible, typically with the starting time or stopping time of the EARLINET performed measurement time window within 90min of the ISS overpass, for the period from February 2015 to September 2016. The results demonstrate the good agreement of the CATS Level 2 backscatter coefficient and EARLINET. Three ISS overpasses close to the EARLINET stations of Leipzig, Germany; Évora, Portugal; and Dushanbe, Tajikistan, are analyzed here to demonstrate the performance of the CATS lidar system under different conditions. The results show that under cloud-free, relative homogeneous aerosol conditions, CATS is in good agreement with EARLINET, independent of daytime and nighttime conditions. CATS low negative biases are observed, partially attributed to the deficiency of lidar systems to detect tenuous aerosol layers of backscatter signal below the minimum detection thresholds; these are biases which may lead to systematic deviations and slight underestimations of the total aerosol optical depth (AOD) in climate studies. In addition, CATS misclassification of aerosol layers as clouds, and vice versa, in cases of coexistent and/or adjacent aerosol and cloud features, occasionally leads to non-representative, unrealistic, and cloud-contaminated aerosol profiles. Regarding solar illumination conditions, low negative biases in CATS backscatter coefficient profiles, of the order of 6.1%, indicate the good nighttime performance of CATS. During daytime, a reduced signal-to-noise ratio by solar background illumination prevents retrievals of weakly scattering atmospheric layers that would otherwise be detectable during nighttime, leading to higher negative biases, of the order of 22.3%. © Author(s) 2019.
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    Detection and attribution of aerosol-cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic model
    (Katlenburg-Lindau : EGU, 2020) Costa-Surós, Montserrat; Sourdeval, Odran; Acquistapace, Claudia; Baars, Holger; Carbajal Henken, Cintia; Genz, Christa; Hesemann, Jonas; Jimenez, Cristofer; König, Marcel; Kretzschmar, Jan; Madenach, Nils; Meyer, Catrin I.; Schrödner, Roland; Seifert, Patric; Senf, Fabian; Brueck, Matthias; Cioni, Guido; Engels, Jan Frederik; Fieg, Kerstin; Gorges, Ksenia; Heinze, Rieke; Kumar Siligam, Pavan; Burkhardt, Ulrike; Crewell, Susanne; Hoose, Corinna; Seifert, Axel; Tegen, Ina; Quaas, Johannes
    Clouds and aerosols contribute the largest uncertainty to current estimates and interpretations of the Earth's changing energy budget. Here we use a new-generation large-domain large-eddy model, ICON-LEM (ICOsahedral Non-hydrostatic Large Eddy Model), to simulate the response of clouds to realistic anthropogenic perturbations in aerosols serving as cloud condensation nuclei (CCN). The novelty compared to previous studies is that (i) the LEM is run in weather prediction mode and with fully interactive land surface over a large domain and (ii) a large range of data from various sources are used for the detection and attribution. The aerosol perturbation was chosen as peak-aerosol conditions over Europe in 1985, with more than fivefold more sulfate than in 2013. Observational data from various satellite and ground-based remote sensing instruments are used, aiming at the detection and attribution of this response. The simulation was run for a selected day (2 May 2013) in which a large variety of cloud regimes was present over the selected domain of central Europe. It is first demonstrated that the aerosol fields used in the model are consistent with corresponding satellite aerosol optical depth retrievals for both 1985 (perturbed) and 2013 (reference) conditions. In comparison to retrievals from groundbased lidar for 2013, CCN profiles for the reference conditions were consistent with the observations, while the ones for the 1985 conditions were not. Similarly, the detection and attribution process was successful for droplet number concentrations: the ones simulated for the 2013 conditions were consistent with satellite as well as new ground-based lidar retrievals, while the ones for the 1985 conditions were outside the observational range. For other cloud quantities, including cloud fraction, liquid water path, cloud base altitude and cloud lifetime, the aerosol response was small compared to their natural vari ability. Also, large uncertainties in satellite and ground-based observations make the detection and attribution difficult for these quantities. An exception to this is the fact that at a large liquid water path value (LWP > 200 g m-2), the control simulation matches the observations, while the perturbed one shows an LWP which is too large. The model simulations allowed for quantifying the radiative forcing due to aerosol-cloud interactions, as well as the adjustments to this forcing. The latter were small compared to the variability and showed overall a small positive radiative effect. The overall effective radiative forcing (ERF) due to aerosol-cloud interactions (ERFaci) in the simulation was dominated thus by the Twomey effect and yielded for this day, region and aerosol perturbation-2:6 W m-2. Using general circulation models to scale this to a global-mean present-day vs. pre-industrial ERFaci yields a global ERFaci of-0:8 W m-2 © 2020 Author(s).
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    Sun photometer retrievals of Saharan dust properties over Barbados during SALTRACE
    (Katlenburg-Lindau : EGU, 2019) Toledano, Carlos; Torres, Benjamín; Velasco-Merino, Cristian; Althausen, Dietrich; Groß, Silke; Wiegner, Matthias; Weinzierl, Bernadett; Gasteiger, Josef; Ansmann, Albert; González, Ramiro; Mateos, David; Farrel, David; Müller, Thomas; Haarig, Moritz; Cachorro, Victoria E.
    The Saharan Aerosol Long-Range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June-July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study. © 2019 All rights reserved.
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    Constraining the Twomey effect from satellite observations: Issues and perspectives
    (Katlenburg-Lindau : EGU, 2020) Quaas, Johannes; Arola, Antti; Cairns, Brian; Christensen, Matthew; Deneke, Hartwig; Ekman, Annica M.L.; Feingold, Graham; Fridlind, Ann; Gryspeerdt, Edward; Hasekamp, Otto; Li, Zhanqing; Lipponen, Antti; Ma, Po-Lun; Mülmenstädt, Johannes; Nenes, Athanasios; Penner, Joyce E.; Rosenfeld, Daniel; Schrödner, Roland; Sinclair, Kenneth; Sourdeval, Odran; Stier, Philip; Tesche, Matthias; van Diedenhoven, Bastiaan; Wendisch, Manfred
    The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (1Nd; ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to 1Nd; ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, 1Nd; ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of me-Tres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining 1Nd; ant, namely the quantification of (i) the cloud-Active aerosol the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-To-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect. © 2020 BMJ Publishing Group. All rights reserved.
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    The sensitivity of the colour of dust in MSG-SEVIRI Desert Dust infrared composite imagery to surface and atmospheric conditions
    (Göttingen : Copernicus GmbH, 2019) Banks, J.R.; Hünerbein, A.; Heinold, B.; Brindley, H.E.; Deneke, H.; Schepanski, K.
    Infrared "Desert Dust" composite imagery taken by the Spinning Enhanced Visible and InfraRed Imager (SEVIRI), onboard the Meteosat Second Generation (MSG) series of satellites above the equatorial East Atlantic, has been widely used for more than a decade to identify and track the presence of dust storms from and over the Sahara Desert, the Middle East, and southern Africa. Dust is characterised by distinctive pink colours in the Desert Dust false-colour imagery; however, the precise colour is influenced by numerous environmental properties, such as the surface thermal emissivity and skin temperature, the atmospheric water vapour content, the quantity and height of dust in the atmosphere, and the infrared optical properties of the dust itself. For this paper, simulations of SEVIRI infrared measurements and imagery have been performed using a modelling system, which combines dust concentrations simulated by the aerosol transport model COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdelling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model) with radiative transfer simulations from the RTTOV (Radiative Transfer for TOVS) model. Investigating the sensitivity of the synthetic infrared imagery to the environmental properties over a 6-month summertime period from 2011 to 2013, it is confirmed that water vapour is a major control on the apparent colour of dust, obscuring its presence when the moisture content is high. Of the three SEVIRI channels used in the imagery (8.7, 10.8, and 12.0 μm), the channel at 10.8 μm has the highest atmospheric transmittance and is therefore the most sensitive to the surface skin temperature. A direct consequence of this sensitivity is that the background desert surface exhibits a strong diurnal cycle in colour, with light blue colours possible during the day and purple hues prevalent at night. In dusty scenes, the clearest pink colours arise from high-altitude dust in dry atmospheres. Elevated dust influences the dust colour primarily by reducing the contrast in atmospheric transmittance above the dust layer between the SEVIRI channels at 10.8 and 12.0 μm, thereby boosting red and pink colours in the imagery. Hence, the higher the dust altitude, the higher the threshold column moisture needed for dust to be obscured in the imagery: for a sample of dust simulated to have an aerosol optical depth (AOD) at 550 nm of 2-3 at an altitude of 3-4 km, the characteristic colour of the dust may only be impaired when the total column water vapour is particularly moist ('39 mm). Meanwhile, dust close to the surface (altitude < 1 km) is only likely to be apparent when the atmosphere is particularly dry and when the surface is particularly hot, requiring column moisture/13 mm and skin temperatures '314 K, and is highly unlikely to be apparent when the skin temperature is/300 K. Such low-altitude dust will regularly be almost invisible within the imagery, since it will usually be beneath much of the atmospheric water vapour column. It is clear that the interpretation of satellite-derived dust imagery is greatly aided by knowledge of the background environment.
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    Aerosol measurements with a shipborne Sun-sky-lunar photometer and collocated multiwavelength Raman polarization lidar over the Atlantic Ocean
    (Göttingen : Copernicus GmbH, 2019) Yin, Z.; Ansmann, A.; Baars, H.; Seifert, P.; Engelmann, R.; Radenz, M.; Jimenez, C.; Herzog, A.; Ohneiser, K.; Hanbuch, K.; Blarel, L.; Goloub, P.; Victori, S.; Maupin, F.
    A shipborne Sun-sky-lunar photometer of type CE318-T was tested during two trans-Atlantic cruises aboard the German research vessel Polarstern from 54ĝ N to 54ĝ S in May/June and December 2018. The continuous observations of the motion-stabilized shipborne CE318-T enabled the first-time observation of a full diurnal cycle of aerosol optical depth (AOD) and column-mean Ångström coefficient of a mixed dust-smoke episode. The latitudinal distribution of the AOD from the shipborne CE318-T, Raman lidar and MICROTOPS II shows the same trend with highest values in the dust belt from 0 to 20ĝ N and overall low values in the Southern Hemisphere. The linear-regression coefficients of determination between MICROTOPS II and the CE318-T were 0.988, 0.987, 0.994 and 0.994 for AODs at 380, 440, 500 and 870 nm and 0.896 for the Ångström exponent at 440-870 nm. The root-mean-squared differences of AOD at 380, 440, 500 and 870 nm were 0.015, 0.013, 0.010 and 0.009, respectively.
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    Fennec dust forecast intercomparison over the Sahara in June 2011
    (Katlenburg-Lindau : EGU, 2016) Chaboureau, Jean-Pierre; Flamant, Cyrille; Dauhut, Thibaut; Kocha, Cécile; Lafore, Jean-Philippe; Lavaysse, Chistophe; Marnas, Fabien; Mokhtari, Mohamed; Pelon, Jacques; Reinares Martínez, Irene; Schepanski, Kerstin; Tulet, Pierre
    In the framework of the Fennec international programme, a field campaign was conducted in June 2011 over the western Sahara. It led to the first observational data set ever obtained that documents the dynamics, thermodynamics and composition of the Saharan atmospheric boundary layer (SABL) under the influence of the heat low. In support to the aircraft operation, four dust forecasts were run daily at low and high resolutions with convection-parameterizing and convection-permitting models, respectively. The unique airborne and ground-based data sets allowed the first ever intercomparison of dust forecasts over the western Sahara. At monthly scale, large aerosol optical depths (AODs) were forecast over the Sahara, a feature observed by satellite retrievals but with different magnitudes. The AOD intensity was correctly predicted by the high-resolution models, while it was underestimated by the low-resolution models. This was partly because of the generation of strong near-surface wind associated with thunderstorm-related density currents that could only be reproduced by models representing convection explicitly. Such models yield emissions mainly in the afternoon that dominate the total emission over the western fringes of the Adrar des Iforas and the Aïr Mountains in the high-resolution forecasts. Over the western Sahara, where the harmattan contributes up to 80 % of dust emission, all the models were successful in forecasting the deep well-mixed SABL. Some of them, however, missed the large near-surface dust concentration generated by density currents and low-level winds. This feature, observed repeatedly by the airborne lidar, was partly forecast by one high-resolution model only.
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    Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model
    (Katlenburg-Lindau : EGU, 2015) Kim, P.S.; Jacob, D.J.; Fisher, J.A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R.M.; Sulprizio, M.P.; Jimenez, J.L.; Campuzano-Jost, P.; Froyd, K.D.; Liao, J.; Hair, J.W.; Fenn, M.A.; Butler, C.F.; Wagner, N.L.; Gordon, T.D.; Welti, A.; Wennberg, P.O.; Crounse, J.D.; St. Clair, J.M.; Teng, A.P.; Millet, D.B.; Schwarz, J.P.; Markovic, M.Z.; Perring, A.E.
    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer–fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5–3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42−] + [NO3−]) is only 0.5–0.7 mol mol−1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8–28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.