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>

Sulfur hexafluoride (SF6) emissions in East Asia determined by inverse modeling

Fang, X.,Thompson, R. L.,Saito, T.,Yokouchi, Y.,Kim, J.,Li, S.,Kim, K. R.,Park, S.,Graziosi, F.,Stohl, A. Copernicus GmbH 2014 Atmospheric chemistry and physics Vol.14 No.9

<P>Abstract. Sulfur hexafluoride (SF6) has a global warming potential of around 22 800 over a 100-year time horizon and is one of the greenhouse gases regulated under the Kyoto Protocol. Around the year 2000 there was a reversal in the global SF6 emission trend, from a decreasing to an increasing trend, which was likely caused by increasing emissions in countries that are not obligated to report their annual emissions to the United Nations Framework Convention on Climate Change. In this study, SF6 emissions during the period 2006-2012 for all East Asian countries - including Mongolia, China, Taiwan, North Korea, South Korea and Japan - were determined by using inverse modeling and in situ atmospheric measurements. We found that the most important sources of uncertainty associated with these inversions are related to the choice of a priori emissions and their assumed uncertainty, the station network as well as the meteorological input data. Much lower uncertainties are due to seasonal variability in the emissions, inversion geometry and resolution, and the measurement calibration scale. Based on the results of these sensitivity tests, we estimate that the total SF6 emission in East Asia increased rapidly from 2404 ± 325 Mg yr−1 in 2006 to 3787 ± 512 Mg yr−1 in 2009 and stabilized thereafter. China contributed 60-72% to the total East Asian emission for the different years, followed by South Korea (8-16%), Japan (5-16%) and Taiwan (4-7%), while the contributions from North Korea and Mongolia together were less than 3% of the total. The per capita SF6 emissions are highest in South Korea and Taiwan, while the per capita emissions for China, North Korea and Japan are close to global average. During the period 2006-2012, emissions from China and from South Korea increased, while emissions from Taiwan and Japan decreased overall. </P>

On the possibilities to use atmospheric reanalyses to evaluate the warming structure in the Arctic

Chung, C. E.,Cha, H.,Vihma, T.,Rä,isä,nen, P.,Decremer, D. Copernicus GmbH 2013 Atmospheric chemistry and physics Vol.13 No.22

<P>Abstract. There has been growing interest in the vertical structure of the recent Arctic warming. We investigated temperatures at the surface, 925, 700, 500 and 300 hPa levels in the Arctic (north of 70° N) using observations and four reanalyses: ERA-Interim, CFSR, MERRA and NCEP II. For the period 1979-2011, the layers at 500 hPa and below show a warming trend in all seasons in all the chosen reanalyses and observations. Restricting the analysis to the 1998-2011 period, however, all the reanalyses show a cooling trend in the Arctic-mean 500 hPa temperature in autumn, and this also applies to both observations and the reanalyses when restricting the analysis to the locations with available IGRA radiosoundings. During this period, the surface observations mainly representing land areas surrounding the Arctic Ocean reveal no summertime trend, in contrast with the reanalyses whether restricted to the locations of the available surface observations or not. In evaluating the reanalyses with observations, we find that the reanalyses agree better with each other at the available IGRA sounding locations than for the Arctic average, perhaps because the sounding observations were assimilated into reanalyses. Conversely, using the reanalysis data only from locations matching available surface (air) temperature observations does not improve the agreement between the reanalyses. At 925 hPa, CFSR deviates from the other three reanalyses, especially in summer after 2000, and it also deviates more from the IGRA radiosoundings than the other reanalyses do. The CFSR error in summer T925 is due mainly to underestimations in the Canadian-Atlantic sector between 120° W and 0°. The other reanalyses also have negative biases in this longitude band. </P>

The Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI): design, execution, and early results

Piters, A. J. M.,Boersma, K. F.,Kroon, M.,Hains, J. C.,Van Roozendael, M.,Wittrock, F.,Abuhassan, N.,Adams, C.,Akrami, M.,Allaart, M. A. F.,Apituley, A.,Beirle, S.,Bergwerff, J. B.,Berkhout, A. J. C. Copernicus GmbH 2012 Atmospheric measurement techniques Vol.5 No.2

<P><p><strong>Abstract.</strong> From June to July 2009 more than thirty different in-situ and remote sensing instruments from all over the world participated in the Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). The campaign took place at KNMI's Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands. Its main objectives were to determine the accuracy of state-of-the-art ground-based measurement techniques for the detection of atmospheric nitrogen dioxide (both in-situ and remote sensing), and to investigate their usability in satellite data validation. The expected outcomes are recommendations regarding the operation and calibration of such instruments, retrieval settings, and observation strategies for the use in ground-based networks for air quality monitoring and satellite data validation. Twenty-four optical spectrometers participated in the campaign, of which twenty-one had the capability to scan different elevation angles consecutively, the so-called Multi-axis DOAS systems, thereby collecting vertical profile information, in particular for nitrogen dioxide and aerosol. Various in-situ samplers and lidar instruments simultaneously characterized the variability of atmospheric trace gases and the physical properties of aerosol particles. A large data set of continuous measurements of these atmospheric constituents has been collected under various meteorological conditions and air pollution levels. Together with the permanent measurement capability at the CESAR site characterizing the meteorological state of the atmosphere, the CINDI campaign provided a comprehensive observational data set of atmospheric constituents in a highly polluted region of the world during summertime. First detailed comparisons performed with the CINDI data show that slant column measurements of NO₂, O₄ and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO₂ derived from several independent instruments agree within 25% of one another, and MAX-DOAS aerosol optical thickness agrees within 20-30% with AERONET data. For the in-situ NO₂ instrument using a molybdenum converter, a bias was found as large as 5 ppbv during day time, when compared to the other in-situ instruments using photolytic converters.</p> </P>

Structure of forecast error covariance in coupled atmosphere-chemistry data assimilation

Park, S. K.,Lim, S.,Zupanski, M. Copernicus GmbH 2015 Geoscientific model development Vol.8 No.5

<P><p><strong>Abstract.</strong> In this study, we examined the structure of an ensemble-based coupled atmosphere-chemistry forecast error covariance. The Weather Research and Forecasting (WRF) model coupled with Chemistry (WRF-Chem), a coupled atmosphere-chemistry model, was used to create an ensemble error covariance. The control variable includes both the dynamical and chemistry model variables. A synthetic single observation experiment was designed in order to evaluate the cross-variable components of a coupled error covariance. The results indicate that the coupled error covariance has important cross-variable components that allow a physically meaningful adjustment of all control variables. The additional benefit of the coupled error covariance is that a cross-component impact is allowed; e.g., atmospheric observations can exert an impact on chemistry analysis, and vice versa. Given the realistic structure of ensemble forecast error covariance produced by the WRF-Chem, we anticipate that the ensemble-based coupled atmosphere-chemistry data assimilation will respond similarly to assimilation of real observations.</p> </P>

Hygroscopic properties of NaCl and NaNO3 mixture particles as reacted inorganic sea-salt aerosol surrogates

Gupta, D.,Kim, H.,Park, G.,Li, X.,Eom, H.-J.,Ro, C.-U. Copernicus GmbH 2015 Atmospheric chemistry and physics Vol.15 No.6

<P>Abstract. NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NOx/HNO3, so internally mixed NaCl and NaNO3 aerosol particles can co-exist over a wide range of mixing ratios. Laboratory-generated, micrometer-sized NaCl and NaNO3 mixture particles at 10 mixing ratios (mole fractions of NaCl (XNaCl) = 0.1 to 0.9) were examined systematically to observe their hygroscopic behavior, derive experimental phase diagrams for deliquescence and efflorescence, and understand the efflorescence mechanism. During the humidifying process, aerosol particles with the eutonic composition (XNaCl = 0.38) showed only one phase transition at their mutual deliquescence relative humidity (MDRH) of 67.9 (±0.5)% On the other hand, particles with other mixing ratios showed two distinct deliquescence transitions; i.e., the eutonic component dissolved at MDRH, and the remainder in the solid phase dissolved completely at their DRHs depending on the mixing ratios, resulting in a phase diagram composed of four different phases, as predicted thermodynamically. During the dehydration process, NaCl-rich particles (XNaCl > 0.38) showed a two stage efflorescence transition: the first stage was purely driven by the homogeneous nucleation of NaCl and the second stage at the mutual efflorescence RH (MERH) of the eutonic components, with values in the range of 30.0-35.5%. Interestingly, aerosol particles with the eutonic composition (XNaCl = 0.38) also showed two-stage efflorescence, with NaCl crystallizing first followed by heterogeneous nucleation of the remaining NaNO3 on the NaCl seeds. NaNO3-rich particles (XNaCl ≤ 0.3) underwent single-stage efflorescence transitions at ERHs progressively lower than the MERH because of the homogeneous nucleation of NaCl and the almost simultaneous heterogeneous nucleation of NaNO3 on the NaCl seeds. SEM/EDX elemental mapping indicated that the effloresced NaCl-NaNO3 particles at all mixing ratios were composed of a homogeneously crystallized NaCl moiety in the center, surrounded either by the eutonic component (for XNaCl > 0.38) or NaNO3 (for XNaCl ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of pure salts (NaCl or NaNO3 in NaCl- or NaNO3-rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl-NaNO3 mixture aerosol particles can maintain an aqueous phase over a wider RH range than pure NaCl particles as SSA surrogate, making their heterogeneous chemistry more probable. </P>

Contribution of ammonium nitrate to aerosol optical depth and direct radiative forcing by aerosols over East Asia

Park, R. S.,Lee, S.,Shin, S.-K.,Song, C. H. Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.4

<P>Abstract. This study focused on the contribution of ammonium nitrate (NH4NO3) to aerosol optical depth (AOD) and direct radiative forcing (DRF) by aerosols over an East Asian domain. In order to evaluate the contribution, chemistry-transport model (CTM)-estimated AOD was combined with satellite-retrieved AOD, utilizing a data assimilation technique, over East Asia for the entire year of 2006. Using the assimilated AOD and CTM-estimated aerosol optical properties, the DRF by aerosols was estimated over East Asia via a radiative transfer model (RTM). Both assimilated AOD and estimated DRF values showed relatively good agreements with AOD and DRF by aerosols from AERONET. Based on these results, the contributions of NH4NO3 to AOD and DRF by aerosols (ΦAOD and ΦDRF) were estimated for the four seasons of 2006 over East Asia. Both ΦAOD and ΦDRF showed seasonal variations over East Asia within the ranges between 4.7% (summer) and 31.3% (winter) and between 4.7% (summer) and 30.7% (winter), respectively, under clear-sky conditions, showing annual average contributions of 15.6% and 15.3%. Under all-sky conditions, ΦDRF varied between 3.6% (summer) and 24.5% (winter), showing annual average contribution of 12.1% over East Asia. These annual average contributions of NH4NO3 to AOD and DRF are almost comparable to the annual average mass fractions of NH4NO3 in PM2.5 and PM10 (17.0% and 14.0%, respectively). ΦAOD and ΦDRF were even larger in the locations where NH3 and NOx emission rates are strong, such as the central East China (CEC) region and Sichuan Basin. For example, under clear-sky conditions, both ΦAOD and ΦDRF over the CEC region range between 6.9% (summer) and 47.9% (winter) and between 6.7% (summer) and 47.5% (winter), respectively. Based on this analysis, it was concluded that both ΦAOD and ΦDRF cannot be ignored in East Asian air quality and radiative forcing studies, particularly during winter. </P>

An evaluation of ozone dry deposition simulations in East Asia

Park, R. J.,Hong, S. K.,Kwon, H.-A.,Kim, S.,Guenther, A.,Woo, J.-H.,Loughner, C. P. Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.15

<P>Abstract. We use a 3-D regional atmospheric chemistry transport model (WRF-Chem) to examine ozone dry deposition in East Asia, which is an important but uncertain research area because of insufficient observation and numerical studies focusing on East Asia. Here we compare two widely used dry deposition parameterization schemes, the Wesely and M3DRY schemes, which are used in the WRF-Chem and Community Multiscale Air Quality (CMAQ) models, respectively. Simulated ozone dry deposition velocities with the two schemes under identical meteorological conditions show considerable differences (a factor of 2) owing to surface resistance parameterization discrepancies. Resulting ozone concentrations differ by up to 10 ppbv for a monthly mean in May when the peak ozone typically occurs in East Asia. An evaluation of the simulated dry deposition velocities shows that the Wesely scheme calculates values with more pronounced diurnal variation than the M3DRY and results in a good agreement with the observations. However, we find significant changes in simulated ozone concentrations using the Wesely scheme but with different surface type data sets, indicating the high sensitivity of ozone deposition calculations to the input data. The need is high for observations to constrain the dry deposition parameterization and its input data to improve the use of air quality models for East Asia. </P>

Extensive spatiotemporal analyses of surface ozone and related meteorological variables in South Korea for the period 1999-2010

Seo, J.,Youn, D.,Kim, J. Y.,Lee, H. Copernicus GmbH 2014 Atmospheric Chemistry and Physics Vol.14 No.12

<P>Abstract. Spatiotemporal characteristics of surface ozone (O3) variations over South Korea are investigated with consideration of meteorological factors and timescales based on the Kolmogorov-Zurbenko filter (KZ filter), using measurement data at 124 air quality monitoring sites and 72 weather stations for the 12 yr period of 1999-2010. In general, O3 levels at coastal cities are high due to dynamic effects of the sea breeze while those at the inland and Seoul Metropolitan Area (SMA) cities are low due to the NOx titration by local precursor emissions. We examine the meteorological influences on O3 using a combined analysis of the KZ filter and linear regressions between O3 and meteorological variables. We decomposed O3 time series at each site into short-term, seasonal, and long-term components by the KZ filter and regressed on meteorological variables. Impact of temperature on the O3 levels is significantly high in the highly populated SMA and inland region, but low in the coastal region. In particular, the probability of high O3 occurrence doubles with 4 °C of temperature increase in the SMA during high O3 months (May-October). This implies that those regions will experience frequent high O3 events in a future warming climate. In terms of short-term variation, the distribution of high O3 probability classified by wind direction shows the effect of both local precursor emissions and long-range transport from China. In terms of long-term variation, the O3 concentrations have increased by +0.26 ppbv yr−1 (parts per billion by volume) on nationwide average, but their trends show large spatial variability. Singular value decomposition analyses further reveal that the long-term temporal evolution of O3 is similar to that of nitrogen dioxide, although the spatial distribution of their trends is different. This study will be helpful as a reference for diagnostics and evaluation of regional- and local-scale O3 and climate simulations, and as a guide to appropriate O3 control policy in South Korea. </P>

A study on the aerosol optical properties over East Asia using a combination of CMAQ-simulated aerosol optical properties and remote-sensing data via a data assimilation technique

Park, R. S.,Song, C. H.,Han, K. M.,Park, M. E.,Lee, S.-S.,Kim, S.-B.,Shimizu, A. Copernicus GmbH 2011 Atmospheric Chemistry and Physics Vol.11 No.23

<P>Abstract. To more accurately estimate direct radiative forcing (DRF) by aerosols, and better investigate particulate pollution over East Asia, precise calculations of the optical properties of aerosols, such as aerosol optical depth (AOD), single scattering albedo (SSA) and aerosol extinction coefficient (σext), are of primary importance. The aerosol optical properties over East Asia were investigated in this study, based on US EPA Models-3/CMAQ v4.5.1 model simulations. The CMAQ model simulations in this study were improved in several ways compared to those in a previous study (Song et al., 2008). Although the details of the improvements were described in the manuscript, the following points should be emphasized: (1) two data assimilation techniques were employed for producing more accurate AOD products and meteorological fields over East Asia; (2) updated/upgraded emission inventories were used in the CMAQ model simulations with a fine grid resolution of 30 × 30 km2; and (3) the 4-D particulate composition calculated from the CMAQ model simulations was converted into 3-D or 4-D aerosol optical products, using the Malm and Hand (2007) algorithm with significant further modifications. The results from the CMAQ model simulations (without assimilation) showed great improvements compared to those from a previous study. For example, in terms of the regression coefficients (R), R values were increased from 0.48-0.68 (previous study) to 0.62-0.79 (this study). The monthly-averaged CMAQ-simulated single scattering albedo (SSA) also agreed well with the AERONET SSA, with the exceptions of the Hong Kong and Taipei sites, where the air qualities were strongly influenced by active biomass burning events from January to April. There were also excellent matches between the vertical profiles of the CMAQ-simulated σext and LIDAR-retrieved σext. It was also found that the contributions of (NH4)2SO4 during summer, NH4NO3 during winter, sea-salt particles during winter and dust particles during spring to the total AOD were large over East Asia. In particular, the largest contribution of NH4NO3 to the total AOD was found over East Asia during winter. Therefore, it was suggested that this contribution of NH4NO3 should not be neglected. In order to produce more accurate AOD products, the CMAQ-simulated AODs were further assimilated with the MODIS-retrieved AODs. Both of the assimilated and AERONET AODs were better correlated with each other than the CMAQ-simulated and AERONET AODs. The obvious benefits from this study would be that with these improved aerosol optical properties, the particulate pollution (e.g. AOD can be served as a proxy to PM2.5 or PM10) and DRF by aerosols over East Asia can be more satisfactorily investigated in future. </P>