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  • Open Access English
    Authors: 
    Kaltsonoudis, Christos; Jorga, Spiro D.; Louvaris, Evangelos; Florou, Kalliopi; Pandis, Spyros N.;
    Project: EC | EUROCHAMP-2020 (730997), EC | ATMOPACS (267099)

    Smog chamber experiments using ambient air as a starting point can improve our understanding of the evolution of atmospheric particulate matter at timescales longer than those achieved by traditional laboratory experiments. These types of studies can take place under more realistic environmental conditions addressing the interactions among multiple pollutants. The use of two identical smog chambers, with the first serving as the baseline chamber and the second as the perturbation chamber (in which addition or removal of pollutants, addition of oxidants, change in the relative humidity, etc.), can facilitate the interpretation of the results in such inherently complex experiments. The differences of the measurements in the two chambers can be used as the basis for the analysis of the corresponding chemical or physical processes of ambient air. A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers (1.5 m3 each). The two chambers are surrounded by UV lamps in a hexagonal arrangement yielding a total JNO2 of 0.1 min−1. The system can be easily disassembled and transported, enabling the study of various atmospheric environments. Moreover, it can be used with natural sunlight. The results of test experiments using ambient air as the starting point are discussed as examples of applications of this system.

  • Open Access English
    Authors: 
    Karnezi, E.; Riipinen, I.; Pandis, S. N.;
    Project: EC | ATMOPACS (267099)

    Organic compounds represent a significant fraction of submicrometer atmospheric aerosol mass. Even if most of these compounds are semi-volatile in atmospheric concentrations, the ambient organic aerosol volatility is quite uncertain. The most common volatility measurement method relies on the use of a thermodenuder (TD). The aerosol passes through a heated tube where its more volatile components evaporate, leaving the less volatile components behind in the particulate phase. The typical result of a thermodenuder measurement is the mass fraction remaining (MFR), which depends, among other factors, on the organic aerosol (OA) vaporization enthalpy and the accommodation coefficient. We use a new method combining forward modeling, introduction of "experimental" error, and inverse modeling with error minimization for the interpretation of TD measurements. The OA volatility distribution, its effective vaporization enthalpy, the mass accommodation coefficient and the corresponding uncertainty ranges are calculated. Our results indicate that existing TD-based approaches quite often cannot estimate reliably the OA volatility distribution, leading to large uncertainties, since there are many different combinations of the three properties that can lead to similar thermograms. We propose an improved experimental approach combining TD and isothermal dilution measurements. We evaluate this experimental approach using the same model, and show that it is suitable for studies of OA volatility in the lab and the field.

  • Open Access English
    Authors: 
    Heckel, A.; Kim, S.-W.; Frost, G. J.; Richter, A.; Trainer, M.; Burrows, J. P.;
    Project: EC | CITYZEN (212095)

    The retrieval of tropospheric columns of NO2 and other trace gases from satellite observations of backscattered solar radiation relies on the use of accurate a priori information. The spatial resolution of current space sensors is often significantly higher than that of the a priori datasets used, introducing uncertainties from spatial misrepresentation. In this study, the effect of spatial under-sampling of a priori data on the retrieval of NO2 columns was studied for a typical coastal area (around San Francisco). High-resolution (15 × 15 km2) NO2 a priori data from the WRF-Chem model in combination with high-resolution MODIS surface reflectance and aerosol data were used to investigate the uncertainty introduced by applying a priori data at typical global chemical transport model resolution. The results show that the relative uncertainties can be large (more than a factor of 2 if all a priori data used is at the coarsest resolution) for individual measurements, mainly due to spatial variations in NO2 profile and surface albedo, with smaller contributions from aerosols and surface height changes. Similar sensitivities are expected for other coastal regions and localised sources such as power plants, highlighting the need for high-resolution a priori data in quantitative analysis of the spatial patterns retrieved from satellite observations of tropospheric pollution.

  • Open Access English
    Authors: 
    Roscoe, H. K.; Roozendael, M.; Fayt, C.; Piesanie, A.; Abuhassan, N.; Adams, C.; Akrami, M.; Cede, A.; Chong, J.; Clémer, K.; +41 more
    Project: EC | MEGAPOLI (212520)

    In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97° N, 4.93° E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose non-zenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO2 and O4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO2, as previous intercomparisons were only for zenith instruments focussing on stratospheric NO2, with their longer heritage.

Advanced search in
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arrow_drop_down
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4 Research products, page 1 of 1
  • Open Access English
    Authors: 
    Kaltsonoudis, Christos; Jorga, Spiro D.; Louvaris, Evangelos; Florou, Kalliopi; Pandis, Spyros N.;
    Project: EC | EUROCHAMP-2020 (730997), EC | ATMOPACS (267099)

    Smog chamber experiments using ambient air as a starting point can improve our understanding of the evolution of atmospheric particulate matter at timescales longer than those achieved by traditional laboratory experiments. These types of studies can take place under more realistic environmental conditions addressing the interactions among multiple pollutants. The use of two identical smog chambers, with the first serving as the baseline chamber and the second as the perturbation chamber (in which addition or removal of pollutants, addition of oxidants, change in the relative humidity, etc.), can facilitate the interpretation of the results in such inherently complex experiments. The differences of the measurements in the two chambers can be used as the basis for the analysis of the corresponding chemical or physical processes of ambient air. A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers (1.5 m3 each). The two chambers are surrounded by UV lamps in a hexagonal arrangement yielding a total JNO2 of 0.1 min−1. The system can be easily disassembled and transported, enabling the study of various atmospheric environments. Moreover, it can be used with natural sunlight. The results of test experiments using ambient air as the starting point are discussed as examples of applications of this system.

  • Open Access English
    Authors: 
    Karnezi, E.; Riipinen, I.; Pandis, S. N.;
    Project: EC | ATMOPACS (267099)

    Organic compounds represent a significant fraction of submicrometer atmospheric aerosol mass. Even if most of these compounds are semi-volatile in atmospheric concentrations, the ambient organic aerosol volatility is quite uncertain. The most common volatility measurement method relies on the use of a thermodenuder (TD). The aerosol passes through a heated tube where its more volatile components evaporate, leaving the less volatile components behind in the particulate phase. The typical result of a thermodenuder measurement is the mass fraction remaining (MFR), which depends, among other factors, on the organic aerosol (OA) vaporization enthalpy and the accommodation coefficient. We use a new method combining forward modeling, introduction of "experimental" error, and inverse modeling with error minimization for the interpretation of TD measurements. The OA volatility distribution, its effective vaporization enthalpy, the mass accommodation coefficient and the corresponding uncertainty ranges are calculated. Our results indicate that existing TD-based approaches quite often cannot estimate reliably the OA volatility distribution, leading to large uncertainties, since there are many different combinations of the three properties that can lead to similar thermograms. We propose an improved experimental approach combining TD and isothermal dilution measurements. We evaluate this experimental approach using the same model, and show that it is suitable for studies of OA volatility in the lab and the field.

  • Open Access English
    Authors: 
    Heckel, A.; Kim, S.-W.; Frost, G. J.; Richter, A.; Trainer, M.; Burrows, J. P.;
    Project: EC | CITYZEN (212095)

    The retrieval of tropospheric columns of NO2 and other trace gases from satellite observations of backscattered solar radiation relies on the use of accurate a priori information. The spatial resolution of current space sensors is often significantly higher than that of the a priori datasets used, introducing uncertainties from spatial misrepresentation. In this study, the effect of spatial under-sampling of a priori data on the retrieval of NO2 columns was studied for a typical coastal area (around San Francisco). High-resolution (15 × 15 km2) NO2 a priori data from the WRF-Chem model in combination with high-resolution MODIS surface reflectance and aerosol data were used to investigate the uncertainty introduced by applying a priori data at typical global chemical transport model resolution. The results show that the relative uncertainties can be large (more than a factor of 2 if all a priori data used is at the coarsest resolution) for individual measurements, mainly due to spatial variations in NO2 profile and surface albedo, with smaller contributions from aerosols and surface height changes. Similar sensitivities are expected for other coastal regions and localised sources such as power plants, highlighting the need for high-resolution a priori data in quantitative analysis of the spatial patterns retrieved from satellite observations of tropospheric pollution.

  • Open Access English
    Authors: 
    Roscoe, H. K.; Roozendael, M.; Fayt, C.; Piesanie, A.; Abuhassan, N.; Adams, C.; Akrami, M.; Cede, A.; Chong, J.; Clémer, K.; +41 more
    Project: EC | MEGAPOLI (212520)

    In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97° N, 4.93° E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose non-zenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO2 and O4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO2, as previous intercomparisons were only for zenith instruments focussing on stratospheric NO2, with their longer heritage.

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