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  • Total column ozone variations over oceanic region around Indian sub-continent during pre-monsoon of 2006

    Special campaign mode ship-based sun photometric observations of total column ozone over the oceanic regions around the Indian sub-continent (56° E–6° E, 4° N–° N) during the pre-monsoon period (18 March–11 May) of 2006 have been used to investigate the spatial and temporal distributions. The overall mean ozone content over the sea region during this period is 298 DU with a variability of ±10 DU. There is a well defined diurnal (daytime) variation in total column ozone with maximum content around the noon-time hours. The amplitude of diurnal variation is higher over the Arabian Sea compared to that over Bay of Bengal. Spatial distribution of total ozone shows higher values over the Head Bay (North Bay of Bengal) and all along the west coast of India strongly pointing to continental origin of possible anthropogenic source. This is further corroborated from the spatial distribution of simultaneously measured aerosol optical thickness (AOT, at 1020 nm) and precipitable water. The overall mean AOT over the oceanic region is 0.09 and mean precipitable water (water vapor) over Indian Ocean region was 3.25 cm which is almost 1 cm higher than that observed over Bay of Bengal and Arabian Sea during the above pre-monsoon period.
  • Development and evaluation of an operational SDS forecasting system for East Asia: CUACE/Dust

    CUACE/Dust, an operational mesoscale sand and dust storm (SDS) forecasting system for East Asia, has been developed by online coupling a dust aerosol emission scheme and dust aerosol microphysics onto a regional meteorological model with improved advection and diffusion schemes and a detailed Northeast Asia soil erosion database. With improved initial dust aerosol conditions through a 3-DVar data assimilation system, CUACE/Dust successfully forecasted most of the 31 SDS processes in East Asia. A detailed comparison of the model predictions for the 8–12 March SDS process with surface network observations and lidar measurements revealed a robust forecasting ability of the system. The time series of the operationally forecasted dust concentrations for a number of representative stations for the whole spring 2006 (1 March–31 May) were evaluated against surface PM10 monitoring data, showing a good agreement in terms of the SDS timing and magnitudes at and near the source regions where dust aerosols dominate. For the operational forecasts of spring 2006 in East Asia, a TS (threat score) system evaluated the performance of CUACE/Dust against all available observations and rendered a spring averaged TS value of 0.31 for FT1 (24 h forecasts), 0.23 for FT2 (48 h forecasts) and 0.21 for FT3 (72 h forecasts).
  • Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol

    In this study, we characterize the CCN activity of the water-soluble organics in biomass burning aerosol. The aerosol after collection upon filters is dissolved in water using sonication. Hydrophobic and hydrophilic components are fractionated from a portion of the original sample using solid phase extraction, and subsequently desalted. The surface tension and CCN activity of these different samples are measured with a KSV CAM 200 goniometer and a DMT Streamwise Thermal Gradient CCN Counter, respectively. The measurements show that the strongest surfactants are isolated in the hydrophobic fraction, while the hydrophilics exhibit negligible surface tension depression. The presence of salts (primarily (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>) in the hydrophobic fraction substantially enhances surface tension depression; their synergistic effects considerably enhance CCN activity, exceeding that of pure (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>. From our analysis, average thermodynamic properties (i.e, molar volume) are determined for samples using our newly developed Köhler Theory Analysis (KTA) method. The molar mass of the hydrophilic and hydrophobic aerosol components is estimated to be 87&plusmn;26 g mol<sup>&minus;1</sup> and 780&plusmn;231 g mol<sup>&minus;1</sup>, respectively. KTA also suggests that the relative proportion (in moles) of hydrophobic to hydrophilic compounds in the original sample to be 1:3. For the first time, KTA is applied to an aerosol with this level of complexity and displays its potential for providing physically-based constraints for GCM parameterizations of the aerosol indirect effect.
  • Antarctic network of lamp-calibrated multichannel radiometers for continuous ozone and uv radiation data

    Three NILU-UV multichannel radiometers have been installed in 1999 at the Argentinian sites of Ushuaia (54S), Marambio (64S) and Belgrano-II (77S) in order to continuously monitor UV radiation, photosynthetically active radiation and total ozone. The measurements were established by INM, Spain in collaboration with FMI, Finland, DNA-IAA, Argentina and CADIC, Argentina to observe and characterize the spatial and temporal evolution of ozone and ultraviolet radiation in the Antarctic region. Special attention has been given to the quality control and quality assurance of the measurements under harsh climatological conditions. The ozone and UV time series of 2000&ndash;2006 were calibrated using a polynomial fit for lamp measurements performed every second week all year round. The gaps in these data are minimal, with almost no data missing, and the data products are available from <a href="http://www.polarvortex.org" target="_blank">http://www.polarvortex.org</a> in near real time. The data products include the erythemally-weighted UV, UVB and UVA radiation, photosynthetically active radiation (PAR), total ozone (O<sub>3</sub>) and a cloud parameter (CLT). For UV data, dose rates as well as daily doses are available; from these the maximum measured UV indices (UVI), during 2000&ndash;2006, were 12.0, 9.7 and 8.1 at Ushuaia, Marambio and Belgrano-II, respectively.
  • Long-term climatology of air mass transport through the Tropical Tropopause Layer (TTL) during NH winter

    A long-term climatology of air mass transport through the tropical tropopause layer (TTL) is presented, covering the period from 1962&ndash;2005. The transport through the TTL is calculated with a Lagrangian approach using radiative heating rates as vertical velocities in an isentropic trajectory model. We demonstrate the improved performance of such an approach compared to previous studies using vertical winds from meteorological analyses. Within the upper part of the TTL, the averaged diabatic ascent is 0.5 K/day during Northern Hemisphere (NH) winters 1992&ndash;2001. Climatological maps show a cooling and strengthening of this part of the residual circulation during the 1990s and early 2000s compared to the long-term mean. Lagrangian cold point (LCP) fields show systematic differences for varying time periods and natural forcing components. The interannual variability of LCP temperature and density fields is found to be influenced by volcanic eruptions, El Niño Southern Oscillation (ENSO), Quasi-Biennial Oscillation (QBO) and the solar cycle. The coldest and driest TTL is reached during QBO easterly phase and La Niña over the western Pacific, whereas during volcanic eruptions, El Niño and QBO westerly phase it is warmer and less dry.
  • Airborne measurements of HCl from the marine boundary layer to the lower stratosphere over the North Pacific Ocean during INTEX-B

    Gas phase HCl was measured from the marine boundary layer (MBL) to the lower stratosphere from the NASA DC-8 during five science flights (41 h) of the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B) field campaign. In the upper troposphere/lower stratosphere (UT/LS, 8&ndash;12 km) HCl was observed to range from a few tens to 100 pptv due to stratospheric influence with a background tropospheric level of less than 2 pptv. In the 8&ndash;12 km altitude range, a simple analysis of the O<sub>3</sub>/HCl correlation shows that pure stratospheric and mixed tropospheric/stratospheric air masses were encountered 30% and 15% of the time, respectively. In the mid troposphere (4&ndash;8 km) HCl levels were usually below 2 pptv except for a few cases of stratospheric influence and were much lower than reported in previous work. These data indicate that background levels of HCl in the mid and upper troposphere are very low and confirm its use in these regions as a tracer of stratospheric ozone. However, a case study suggests that HCl may be produced in the mid troposphere by the dechlorination of dust aerosols. In the remote marine boundary layer HCl levels were consistently above 20 pptv (up to 140 pptv) and strongly correlated with HNO<sub>3</sub>. Cl atom levels were estimated from the background level of HCl in the MBL. This analysis suggests a Cl concentration of ~3&times;10<sup>3</sup> atoms cm<sup>&minus;3</sup>, which corresponds to the lower range of previous studies. Finally, the observed HCl levels are compared to predictions by the Real-time Air Quality Modeling System (RAQMS) to assess its ability to characterize the impact of stratospheric transport on the upper troposphere.
  • Intercomparison of ILAS-II version 1.4 and version 2 target parameters with MIPAS-Envisat measurements

    This paper assesses the mean differences between the two ILAS-II data versions (1.4 and 2) by comparing them with MIPAS measurements made between May and October 2003. For comparison with ILAS-II results, MIPAS data processed at the Institut für Meteorologie und Klimaforschung, Karlsruhe, Germany (IMK) in cooperation with the Instituto de Astrofísica de Andalucía (IAA) in Granada, Spain, were used. The coincidence criteria of &plusmn;300 km in space and &plusmn;12 h in time for H<sub>2</sub>O, N<sub>2</sub>O, and CH<sub>4</sub> and the coincidence criteria of &plusmn;300 km in space and &plusmn;6 h in time for ClONO<sub>2</sub>, O<sub>3</sub>, and HNO<sub>3</sub> were used. The ILAS-II data were separated into sunrise (= Northern Hemisphere) and sunset (= Southern Hemisphere). For the sunrise data, a clear improvement from version 1.4 to version 2 was observed for H<sub>2</sub>O, CH<sub>4</sub>, ClONO<sub>2</sub>, and O<sub>3</sub>. In particular, the ILAS-II version 1.4 mixing ratios of H<sub>2</sub>O and CH<sub>4</sub> were unrealistically small, and those of ClONO<sub>2</sub> above altitudes of 30 km unrealistically large. For N<sub>2</sub>O and HNO<sub>3</sub>, there were no large differences between the two versions. Contrary to the Northern Hemisphere, where some exceptional profiles deviated significantly from known climatology, no such outlying profiles were found in the Southern Hemisphere for both versions. Generally, the ILAS-II version 2 data were in better agreement with the MIPAS data than the version 1.4, and are recommended for quantitative analysis in the stratosphere. For H<sub>2</sub>O data in the Southern Hemisphere, further data quality evaluation is necessary.
  • Equatorial wave analysis from SABER and ECMWF temperatures

    Equatorial planetary scale wave modes such as Kelvin waves or Rossby-gravity waves are excited by convective processes in the troposphere. In this paper an analysis for these and other equatorial wave modes is carried out with special focus on the stratosphere using temperature data from the SABER satellite instrument as well as ECMWF temperatures. Space-time spectra of symmetric and antisymmetric spectral power are derived to separate the different equatorial wave types and the contribution of gravity waves is determined from the spectral background of the space-time spectra. <br><br> Both gravity waves and equatorial planetary scale wave modes are main drivers of the quasi-biennial oscillation (QBO) in the stratosphere. Temperature variances attributed to the different wave types are calculated for the period from February 2002 until March 2006 and compared to previous findings. A comparison between SABER and ECMWF wave analyses shows that in the lower stratosphere SABER and ECMWF spectra and temperature variances agree remarkably well while in the upper stratosphere ECMWF tends to overestimate Kelvin wave components. Gravity wave variances are partly reproduced by ECMWF but have a significant low-bias. For the examples of a QBO westerly phase (October&ndash;December 2004) and a QBO easterly phase (November/December 2005, period of the SCOUT-O3 tropical aircraft campaign in Darwin/Australia) in the lower stratosphere we find qualitatively good agreement between SABER and ECMWF in the longitude-time distribution of Kelvin, Rossby (<i>n</i>=1), and Rossby-gravity waves.
  • On the vertical distribution of boundary layer halogens over coastal Antarctica: implications for O3, HOx, NOx and the Hg lifetime

    A one-dimensional chemical transport model has been developed to investigate the vertical gradients of bromine and iodine compounds in the Antarctic coastal boundary layer (BL). The model has been applied to interpret recent year-round observations of iodine and bromine monoxides (IO and BrO) at Halley Station, Antarctica. The model requires an equivalent I atom flux of ~10<sup>10</sup> molecule cm<sup>&minus;2</sup> s<sup>&minus;1</sup> from the snowpack in order to account for the measured IO levels, which are up to 20 ppt during spring. Using the current knowledge of gas-phase iodine chemistry, the model predicts significant gradients in the vertical distribution of iodine species. However, recent ground-based and satellite observations of IO imply that the radical is well-mixed in the Antarctic boundary layer, indicating a longer than expected atmospheric lifetime for the radical. This can be modelled by including photolysis of the higher iodine oxides (I<sub>2</sub>O<sub>2</sub>, I<sub>2</sub>O<sub>3</sub>, I<sub>2</sub>O<sub>4</sub> and I<sub>2</sub>O<sub>5</sub>), and rapid recycling of HOI and INO<sub>3</sub> through sea-salt aerosol. The model also predicts significant concentrations (up to 25 ppt) of I<sub>2</sub>O<sub>5</sub> in the lowest 10 m of the boundary layer. Heterogeneous chemistry involving sea-salt aerosol is also necessary to account for the vertical profile of BrO. Iodine chemistry causes a large increase (typically more than 3-fold) in the rate of O<sub>3</sub> depletion in the BL, compared with bromine chemistry alone. Rapid entrainment of O<sub>3</sub> from the free troposphere appears to be required to account for the observation that on occasion there is little O<sub>3</sub> depletion at the surface in the presence of high concentrations of IO and BrO. The halogens also cause significant changes to the vertical profiles of OH and HO<sub>2</sub> and the NO<sub>2</sub>/NO ratio. The average Hg<sup>0</sup> lifetime against oxidation is also predicted to be about 10 h during springtime. An important result from the model is that very large fluxes of iodine precursors into the boundary layer are required to account for the observed levels of IO. The mechanisms which cause these emissions are unknown. Overall, our results show that halogens profoundly influence the oxidizing capacity of the Antarctic troposphere.
  • Do supersonic aircraft avoid contrails?

    The impact of a potential future fleet of supersonic aircraft on contrail coverage and contrail radiative forcing is investigated by means of simulations with the general circulation model ECHAM4.L39(DLR) including a contrail parameterization. The model simulations consider air traffic inventories of a subsonic fleet and of a combined fleet of sub- and supersonic aircraft for the years 2025 and 2050, respectively. In case of the combined fleet, part of the subsonic fleet is replaced by supersonic aircraft. The combined air traffic scenario reveals a reduction in contrail cover at subsonic cruise levels (10 to 12 km) in the northern extratropics, especially over the North Atlantic and North Pacific. At supersonic flight levels (18 to 20 km), contrail formation is mainly restricted to tropical regions. Only in winter is the northern extratropical stratosphere above the 100 hPa level cold enough for the formation of contrails. Total contrail coverage is only marginally affected by the shift in flight altitude. The model simulations indicate a global annual mean contrail cover of 0.372% for the subsonic and 0.366% for the combined fleet in 2050. The simulated contrail radiative forcing is most closely correlated to the total contrail cover, although contrails in the tropical lower stratosphere are found to be optically thinner than contrails in the extratropical upper troposphere. The global annual mean contrail radiative forcing in 2050 (2025) amounts to 24.7 mW m<sup>&minus;2</sup> (9.4 mW m<sup>&minus;2</sup>) for the subsonic fleet and 24.2 mW m<sup>&minus;2</sup> (9.3 mW m<sup>&minus;2</sup>) for the combined fleet. A reduction of the supersonic cruise speed from Mach 2.0 to Mach 1.6 leads to a downward shift in contrail cover, but does not affect global mean total contrail cover and contrail radiative forcing. Hence the partial substitution of subsonic air traffic leads to a shift of contrail occurrence from mid to low latitudes, but the resulting change in contrail-induced climate impact is almost negligible.
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