Improvement of aerosol optical depth retrieval from MODIS spectral reflectance over the global ocean using new aerosol models archived from AERONET inversion data and tri-axial ellipsoidal dust database

Lee, J.,Kim, J.,Yang, P.,Hsu, N. C. Copernicus GmbH 2012 Atmospheric chemistry and physics Vol.12 No.15

<P>Abstract. New over-ocean aerosol models are developed by integrating the inversion data from the Aerosol Robotic Network (AERONET) sun/sky radiometers with a database for the optical properties of tri-axial ellipsoid particles. The new aerosol models allow more accurate retrieval of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) in the case of high AOD (AOD > 0.3). The aerosol models are categorized by using the fine-mode fraction (FMF) at 550 nm and the single-scattering albedo (SSA) at 440 nm from the AERONET inversion data to include a variety of aerosol types found around the globe. For each aerosol model, the changes in the aerosol optical properties (AOPs) as functions of AOD are considered to better represent aerosol characteristics. Comparisons of AODs between AERONET and MODIS for the period from 2003 to 2010 show that the use of the new aerosol models enhances the AOD accuracy with a Pearson coefficient of 0.93 and a regression slope of 0.99 compared to 0.92 and 0.85 calculated using the MODIS Collection 5 data. Moreover, the percentage of data within an expected error of ± (0.03 + 0.05 × AOD) is increased from 62% to 64% for overall data and from 39% to 5% for AOD > 0.3. Errors in the retrieved AOD are further characterized with respect to the Ångström exponent (AE), scattering angle (Θ), SSA, and air mass factor (AMF). Due to more realistic AOPs assumptions, the new algorithm generally reduces systematic errors in the retrieved AODs compared with the current operational algorithm. In particular, the underestimation of fine-dominated AOD and the scattering angle dependence of dust-dominated AOD are significantly mitigated as results of the new algorithm's improved treatment of aerosol size distribution and dust particle nonsphericity. </P>

Long-term MAX-DOAS network observations of NO2 in Russia and Asia (MADRAS) during the period 2007–2012: instrumentation, elucidation of climatology, and comparisons with OMI satellite observations and global model simulations

Kanaya, Y.,Irie, H.,Takashima, H.,Iwabuchi, H.,Akimoto, H.,Sudo, K.,Gu, M.,Chong, J.,Kim, Y. J.,Lee, H.,Li, A.,Si, F.,Xu, J.,Xie, P.-H.,Liu, W.-Q.,Dzhola, A.,Postylyakov, O.,Ivanov, V.,Grechko, E.,Ter Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.15

<P>Abstract. We conducted long-term network observations using standardized Multi-Axis Differential optical absorption spectroscopy (MAX-DOAS) instruments in Russia and ASia (MADRAS) from 2007 onwards and made the first synthetic data analysis. At seven locations (Cape Hedo, Fukue and Yokosuka in Japan, Hefei in China, Gwangju in Korea, and Tomsk and Zvenigorod in Russia) with different levels of pollution, we obtained 80 927 retrievals of tropospheric NO2 vertical column density (TropoNO2VCD) and aerosol optical depth (AOD). In the technique, the optimal estimation of the TropoNO2VCD and its profile was performed using aerosol information derived from O4 absorbances simultaneously observed at 460-490 nm. This large data set was used to analyze NO2 climatology systematically, including temporal variations from the seasonal to the diurnal scale. The results were compared with Ozone Monitoring Instrument (OMI) satellite observations and global model simulations. Two NO2 retrievals of OMI satellite data (NASA ver. 2.1 and Dutch OMI NO2 (DOMINO) ver. 2.0) generally showed close correlations with those derived from MAX-DOAS observations, but had low biases of up to ~50%. The bias was distinct when NO2 was abundantly present near the surface and when the AOD was high, suggesting a possibility of incomplete accounting of NO2 near the surface under relatively high aerosol conditions for the satellite observations. Except for constant biases, the satellite observations showed nearly perfect seasonal agreement with MAX-DOAS observations, suggesting that the analysis of seasonal features of the satellite data were robust. Weekend reduction in the TropoNO2VCD found at Yokosuka and Gwangju was absent at Hefei, implying that the major sources had different weekly variation patterns. While the TropoNO2VCD generally decreased during the midday hours, it increased exceptionally at urban/suburban locations (Yokosuka, Gwangju, and Hefei) during winter. A global chemical transport model, MIROC-ESM-CHEM (Model for Interdisciplinary Research on Climate-Earth System Model-Chemistry), was validated for the first time with respect to background NO2 column densities during summer at Cape Hedo and Fukue in the clean marine atmosphere. </P>

Hygroscopic properties of newly formed ultrafine particles at an urban site surrounded by deciduous forest (Sapporo, northern Japan) during the summer of 2011

Jung, J.,Kawamura, K. Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.14

<P>Abstract. To investigate the hygroscopic properties of ultrafine particles during new particle formation events, the hygroscopic growth factors of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. The hygroscopic growth factor at 85 % relative humidity [g(85%)] of freshly formed nucleation mode particles was 1.11 to 1.28 (average: 1.16 ± 0.06) at a dry particle diameter (Dp) centered on 20 nm, which is equivalent to 1.17 to 1.35 (1.23 ± 0.06) at a dry Dp centered on 100 nm after considering the Kelvin effect. These values are comparable with those of secondary organic aerosols, suggesting that low-volatility organic vapors are important to the burst of nucleation mode particles. The equivalent g(85%) at a dry Dp of 100 nm for nucleated particles that have grown to Aitken mode sizes (1.24 to 1.34; average: 1.30 ± 0.04) were slightly higher than those of newly formed nucleation mode particles, suggesting that the growth of freshly formed nucleation mode particles to the Aitken mode size can be subjected to condensation of not only low-volatility organic vapors, but also water-soluble inorganic species. Based on this result, and previous measurement of radiocarbon in aerosols, we suggest that the burst of nucleation mode particles and their subsequent growth were highly affected by biogenic organic emissions at this measurement site, which is surrounded by deciduous forest. Gradual increases in mode diameter after the burst of nucleation mode particles were observed under southerly wind conditions, with a dominant contribution of intermediately hygroscopic particles. However, sharp increases in mode diameter were observed when the wind direction shifted to northwesterly or northeasterly, with a sharp increase in the highly hygroscopic particle fraction of the Aitken mode particles, indicating that the hygroscopic growth factor of newly formed particles is perturbed by the local winds that deliver different air masses to the measurement site. </P>

TEM analysis of the internal structures and mineralogy of Asian dust particles and the implications for optical modeling

Jeong, G. Y.,Nousiainen, T. Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.14

<P>Abstract. Mineral dust interacts with incoming/outgoing electromagnetic radiation in the atmosphere. This interaction depends on the microphysical properties of the dust particles, including size, mineral composition, external morphology, and internal structure. Ideally all of these properties should be accounted for in the remote sensing of dust, the modeling of single-scattering properties, and radiative effect assessment. There have been many reports on the microphysical characterizations of mineral dust, but no investigations of the internal structures of individual dust particles. We explored the interiors of Asian dust particles using the combined application of focused ion beam thin-slice preparation and high-resolution transmission electron microscopy. The results showed that individual dust particles consisted of numerous mineral grains, which were organized into several types of internal structure: single and polycrystalline cores of quartz, feldspars, calcite, and amphibole often with oriented clay coatings; individual clay agglomerates of nano-thin clay platelets showing preferred to random orientations common with coarser mineral inclusions; and platy coarse phyllosilicates (muscovite, biotite, and chlorite). Micron to submicron pores were scattered throughout the interior of particles. Clays in the coatings and agglomerates were dominated by nano-thin platelets of the clay minerals of illite-smectite series including illite, smectite, and their mixed layers with subordinate kaolinite and clay-sized chlorite. Submicron iron oxide grains, dominantly goethite, were distributed throughout the clay agglomerates and coatings. Unlike the common assumptions and simplifications, we found that the analyzed dust particles were irregularly shaped with birefringent, polycrystalline, and polymineralic heterogeneous compositions. Accounting for this structural and mineralogical makeup may improve the remote sensing retrieval of dust and the evaluation of radiation effects, but will also require sophisticated single-scattering modeling. In particular, the observed internal structures of dust particles such as clay coatings, preferred orientation, embedded grains in clays, and pores, have the potential to considerably impact on the light scattering by dust particles. The distribution and size of structural components with contrasting dielectric properties, such as iron oxides, should also be explicitly accounted for. </P>

Momentum forcing of the quasi-biennial oscillation by equatorial waves in recent reanalyses

Kim, Y.-H.,Chun, H.-Y. Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.12

<P>Abstract. The momentum forcing of the QBO (quasi-biennial oscillation) by equatorial waves is estimated using recent reanalyses. Based on the estimation using the conventional pressure-level data sets, the forcing by the Kelvin waves (3-9 m s−1 month−1) dominates the net forcing by all equatorial wave modes (3-11 m s−1 month−1) in the easterly-to-westerly transition phase at 30 hPa. In the opposite phase, the net forcing by equatorial wave modes is small (1-5 m s−1 month−1). By comparing the results with those from the native model-level data set of the ERA-Interim reanalysis, it is suggested that the use of conventional-level data causes the Kelvin wave forcing to be underestimated by 2-4 m s−1 month−1. The momentum forcing by mesoscale gravity waves, which are unresolved in the reanalyses, is deduced from the residual of the zonal wind tendency equation. In the easterly-to-westerly transition phase at 30 hPa, the mesoscale gravity wave forcing is found to be smaller than the resolved wave forcing, whereas the gravity wave forcing dominates over the resolved wave forcing in the opposite phase. Finally, we discuss the uncertainties in the wave forcing estimates using the reanalyses. </P>

Ensemble data assimilation of total column ozone using a coupled meteorology-chemistry model and its impact on the structure of Typhoon Nabi (2005)

Lim, S.,Park, S. K.,Zupanski, M. Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.17

<P>Abstract. Ozone (O3) plays an important role in chemical reactions and is usually incorporated in chemical data assimilation (DA). In tropical cyclones (TCs), O3 usually shows a lower concentration inside the eyewall and an elevated concentration around the eye, impacting meteorological as well as chemical variables. To identify the impact of O3 observations on TC structure, including meteorological and chemical information, we developed a coupled meteorology-chemistry DA system by employing the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) and an ensemble-based DA algorithm - the maximum likelihood ensemble filter (MLEF). For a TC case that occurred over East Asia, Typhoon Nabi (2005), our results indicate that the ensemble forecast is reasonable, accompanied with larger background state uncertainty over the TC, and also over eastern China. Similarly, the assimilation of O3 observations impacts meteorological and chemical variables near the TC and over eastern China. The strongest impact on air quality in the lower troposphere was over China, likely due to the pollution advection. In the vicinity of the TC, however, the strongest impact on chemical variables adjustment was at higher levels. The impact on meteorological variables was similar in both over China and near the TC. The analysis results are verified using several measures that include the cost function, root mean square (RMS) error with respect to observations, and degrees of freedom for signal (DFS). All measures indicate a positive impact of DA on the analysis - the cost function and RMS error have decreased by 16.9 and 8.87 %, respectively. In particular, the DFS indicates a strong positive impact of observations in the TC area, with a weaker maximum over northeastern China. </P>

Estimation of PM10 concentrations over Seoul using multiple empirical models with AERONET and MODIS data collected during the DRAGON-Asia campaign

Seo, S.,Kim, J.,Lee, H.,Jeong, U.,Kim, W.,Holben, B. N.,Kim, S.-W.,Song, C. H.,Lim, J. H. Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.1

<P>Abstract. The performance of various empirical linear models to estimate the concentrations of surface-level particulate matter with a diameter less than 10 μm (PM10) was evaluated using Aerosol Robotic Network (AERONET) sun photometer and Moderate-Resolution Imaging Spectroradiometer (MODIS) data collected in Seoul during the Distributed Regional Aerosol Gridded Observation Network (DRAGON)-Asia campaign from March to May 2012. An observed relationship between the PM10 concentration and the aerosol optical depth (AOD) was accounted for by several parameters in the empirical models, including boundary layer height (BLH), relative humidity (RH), and effective radius of the aerosol size distribution (Reff), which was used here for the first time in empirical modeling. Among various empirical models, the model which incorporates both BLH and Reff showed the highest correlation, which indicates the strong influence of BLH and Reff on the PM10 estimations. Meanwhile, the effect of RH on the relationship between AOD and PM10 appeared to be negligible during the campaign period (spring), when RH is generally low in northeast Asia. A large spatial dependency of the empirical model performance was found by categorizing the locations of the collected data into three different site types, which varied in terms of the distances between instruments and source locations. When both AERONET and MODIS data sets were used in the PM10 estimation, the highest correlations between measured and estimated values (R = 0.76 and 0.76 using AERONET and MODIS data, respectively) were found for the residential area (RA) site type, while the poorest correlations (R = 0.61 and 0.68 using AERONET and MODIS data, respectively) were found for the near-source (NS) site type. Significant seasonal variations of empirical model performances for PM10 estimation were found using the data collected at Yonsei University (one of the DRAGON campaign sites) over a period of 17 months including the DRAGON campaign period. The best correlation between measured and estimated PM10 concentrations (R = 0.81) was found in winter, due to the presence of a stagnant air mass and low BLH conditions, which may have resulted in relatively homogeneous aerosol properties within the BLH. On the other hand, the poorest correlation between measured and estimated PM10 concentrations (R = 0.54) was found in spring, due to the influence of the long-range transport of dust to both within and above the BLH. </P>

Variations of surface ozone at Ieodo Ocean Research Station in the East China Sea and the influence of Asian outflows

Han, J.,Shin, B.,Lee, M.,Hwang, G.,Kim, J.,Shim, J.,Lee, G.,Shim, C. Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.21

<P>Abstract. Ieodo Ocean Research Station (IORS), a research tower (~ 40 m a.s.l.) for atmospheric and oceanographic observations, is located in the East China Sea (32.07° N, 125.10° E). The IORS is almost equidistant from South Korea, China, and Japan and, therefore, it is an ideal place to observe Asian outflows without local emission effects. The seasonal variation of ozone was distinct, with a minimum in August (37 ppbv) and two peaks in April and October (62 ppbv), and was largely affected by the seasonal wind pattern over east Asia. At IORS, six types of air masses were distinguished with different levels of O3 concentrations by the cluster analysis of backward trajectories. Marine air masses from the Pacific Ocean represent a relatively clean background air with a lowest ozone level of 32 ppbv, which was most frequently observed in summer (July-August). In spring (March-April) and winter (December-February), the influence of Chinese outflows was dominant with higher ozone concentrations of 62 and 49 ppbv, respectively. This study confirms that the influence of Chinese outflows was the main factor determining O3 levels at IORS and its extent was dependent on meteorological state, particularly at a long-term scale. </P>

The Amazon Tall Tower Observatory (ATTO): overview of pilot measurements on ecosystem ecology, meteorology, trace gases, and aerosols

Andreae, M. O.,Acevedo, O. C.,Araù,jo, A.,Artaxo, P.,Barbosa, C. G. G.,Barbosa, H. M. J.,Brito, J.,Carbone, S.,Chi, X.,Cintra, B. B. L.,da Silva, N. F.,Dias, N. L.,Dias-Jú,nior, C. Q.,Dita Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.18

<P>Abstract. The Amazon Basin plays key roles in the carbon and water cycles, climate change, atmospheric chemistry, and biodiversity. It has already been changed significantly by human activities, and more pervasive change is expected to occur in the coming decades. It is therefore essential to establish long-term measurement sites that provide a baseline record of present-day climatic, biogeochemical, and atmospheric conditions and that will be operated over coming decades to monitor change in the Amazon region, as human perturbations increase in the future. The Amazon Tall Tower Observatory (ATTO) has been set up in a pristine rain forest region in the central Amazon Basin, about 150 km northeast of the city of Manaus. Two 80 m towers have been operated at the site since 2012, and a 325 m tower is nearing completion in mid-2015. An ecological survey including a biodiversity assessment has been conducted in the forest region surrounding the site. Measurements of micrometeorological and atmospheric chemical variables were initiated in 2012, and their range has continued to broaden over the last few years. The meteorological and micrometeorological measurements include temperature and wind profiles, precipitation, water and energy fluxes, turbulence components, soil temperature profiles and soil heat fluxes, radiation fluxes, and visibility. A tree has been instrumented to measure stem profiles of temperature, light intensity, and water content in cryptogamic covers. The trace gas measurements comprise continuous monitoring of carbon dioxide, carbon monoxide, methane, and ozone at five to eight different heights, complemented by a variety of additional species measured during intensive campaigns (e.g., VOC, NO, NO2, and OH reactivity). Aerosol optical, microphysical, and chemical measurements are being made above the canopy as well as in the canopy space. They include aerosol light scattering and absorption, fluorescence, number and volume size distributions, chemical composition, cloud condensation nuclei (CCN) concentrations, and hygroscopicity. In this paper, we discuss the scientific context of the ATTO observatory and present an overview of results from ecological, meteorological, and chemical pilot studies at the ATTO site. </P>

Validation of OMI total ozone retrievals from the SAO ozone profile algorithm and three operational algorithms with Brewer measurements

Bak, J.,Liu, X.,Kim, J. H.,Chance, K.,Haffner, D. P. Copernicus GmbH 2015 Atmospheric Chemistry and Physics Vol.15 No.2

<P>Abstract. The accuracy of total ozone computed from the Smithsonian Astrophysical Observatory (SAO) optimal estimation (OE) ozone profile algorithm (SOE) applied to the Ozone Monitoring Instrument (OMI) is assessed through comparisons with ground-based Brewer spectrometer measurements from 2005 to 2008. We also compare the three OMI operational ozone products, derived from the NASA Total Ozone Mapping Spectrometer (TOMS) algorithm, the KNMI (Royal Netherlands Meteorological Institute) differential optical absorption spectroscopy (DOAS) algorithm, and KNMI's Optimal Estimation (KOE) algorithm. The best agreement is observed between SAO and Brewer, with a mean difference of within 1% at most individual stations. The KNMI OE algorithm systematically overestimates Brewer total ozone by 2% at low and mid-latitudes and 5% at high latitudes while the TOMS and DOAS algorithms underestimate it by ~1.65% on average. Standard deviations of ~1.8% are calculated for both SOE and TOMS, but DOAS and KOE have higher values of 2.2% and 2.6%, respectively. The stability of the SOE algorithm is found to have insignificant dependence on viewing geometry, cloud parameters, or total ozone column. In comparison, the KOE-Brewer differences are significantly correlated with solar and viewing zenith angles and show significant deviations depending on cloud parameters and total ozone amount. The TOMS algorithm exhibits similar stability to SOE with respect to viewing geometry and total column ozone, but has stronger cloud parameter dependence. The dependence of DOAS on observational geometry and geophysical conditions is marginal compared to KOE, but is distinct compared to the SOE and TOMS algorithms. Comparisons of all four OMI products with Brewer show no apparent long-term drift, but seasonal features are evident, especially for KOE and TOMS. The substantial differences in the KOE vs. SOE algorithm performance cannot be sufficiently explained by the use of soft calibration (in SOE) and the use of different a priori error covariance matrices; however, other algorithm details cause fitting residuals larger by a factor of 2-3 for KOE. </P>