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| 2. |
- Hodnebrog, O., et al.
(författare)
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Impact of forest fires, biogenic emissions and high temperatures on the elevated Eastern Mediterranean ozone levels during the hot summer of 2007
- 2012
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8727-8750
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Tidskriftsartikel (refereegranskat)abstract
- The hot summer of 2007 in southeast Europe has been studied using two regional atmospheric chemistry models; WRF-Chem and EMEP MSC-W. The region was struck by three heat waves and a number of forest fire episodes, greatly affecting air pollution levels. We have focused on ozone and its precursors using state-of-the-art inventories for anthropogenic, biogenic and forest fire emissions. The models have been evaluated against measurement data, and processes leading to ozone formation have been quantified. Heat wave episodes are projected to occur more frequently in a future climate, and therefore this study also makes a contribution to climate change impact research. The plume from the Greek forest fires in August 2007 is clearly seen in satellite observations of CO and NO2 columns, showing extreme levels of CO in and downwind of the fires. Model simulations reflect the location and influence of the fires relatively well, but the modelled magnitude of CO in the plume core is too low. Most likely, this is caused by underestimation of CO in the emission inventories, suggesting that the CO/NOx ratios of fire emissions should be re-assessed. Moreover, higher maximum values are seen in WRF-Chem than in EMEP MSC-W, presumably due to differences in plume rise altitudes as the first model emits a larger fraction of the fire emissions in the lowermost model layer. The model results are also in fairly good agreement with surface ozone measurements. Biogenic VOC emissions reacting with anthropogenic NOx emissions are calculated to contribute significantly to the levels of ozone in the region, but the magnitude and geographical distribution depend strongly on the model and biogenic emission module used. During the July and August heat waves, ozone levels increased substantially due to a combination of forest fire emissions and the effect of high temperatures. We found that the largest temperature impact on ozone was through the temperature dependence of the biogenic emissions, closely followed by the effect of reduced dry deposition caused by closing of the plants' stomata at very high temperatures. The impact of high temperatures on the ozone chemistry was much lower. The results suggest that forest fire emissions, and the temperature effect on biogenic emissions and dry deposition, will potentially lead to substantial ozone increases in a warmer climate.
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| 3. |
- Hommel, R., et al.
(författare)
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Chemical ozone loss and ozone mini-hole event during the Arctic winter 2010/2011 as observed by SCIAMACHY and GOME-2
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:7, s. 3247-3276
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Tidskriftsartikel (refereegranskat)abstract
- Record breaking loss of ozone (O-3) in the Arctic stratosphere has been reported in winter-spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O-3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) onboard Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Alesund (78.55 degrees N, 11.55 degrees E). A chemical transport model (CTM) has been used to relate and compare Arctic winter-spring conditions in 2011 with those in the previous year. In late winter-spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O-3 was depleted by halogen catalytic cycles between the 425 and 525K isentropic surfaces, i.e. in the altitude range similar to 16-20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O-3 was removed above the 575K isentrope (similar to 23 km). This loss above 575K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O-3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O-3 around 60 %, previously not discussed in detail, is observed in mid-January 2011 below 500K (similar to 19 km) and sustained for approximately 1 week. The low O-3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.
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| 4. |
- Kerzenmacher, T., et al.
(författare)
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Validation of NO2 and NO from the Atmospheric Chemistry Experiment (ACE)
- 2008
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 8:19, s. 5801--5841-
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Tidskriftsartikel (refereegranskat)abstract
- Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE), using an infrared Fourier Transform Spectrometer (ACE-FTS) and (for NO2) an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation). In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY), stellar occultation measurements (GOMOS), limb measurements (MIPAS, OSIRIS), nadir measurements (SCIAMACHY), balloon-borne measurements (SPIRALE, SAOZ) and ground-based measurements (UV-VIS, FTIR). Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR) profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS) and SAGE II (for ACE-FTS (sunrise) and MAESTRO) and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average) agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.
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| 5. |
- Khosrawi, F., et al.
(författare)
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Sensitivity of polar stratospheric cloud formation to changes in water vapour and temperature
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:1, s. 101-121
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Tidskriftsartikel (refereegranskat)abstract
- More than a decade ago it was suggested that a cooling of stratospheric temperatures by 1 K or an increase of 1 ppmv of stratospheric water vapour could promote denitrification, the permanent removal of nitrogen species from the stratosphere by solid polar stratospheric cloud (PSC) particles. In fact, during the two Arctic winters 2009/10 and 2010/11 the strongest denitrification in the recent decade was observed. Sensitivity studies along air parcel trajectories are performed to test how a future stratospheric water vapour (H2O) increase of 1 ppmv or a temperature decrease of 1K would affect PSC formation. We perform our study based on measurements made during the Arctic winter 2010/11. Air parcel trajectories were calculated 6 days backward in time based on PSCs detected by CALIPSO (Cloud Aerosol Lidar and Infrared Pathfinder satellite observations). The sensitivity study was performed on single trajectories as well as on a trajectory ensemble. The sensitivity study shows a clear prolongation of the potential for PSC formation and PSC existence when the temperature in the stratosphere is decreased by 1K and water vapour is increased by 1 ppmv. Based on 15 years of satellite measurements (20002014) from UARS/HALOE, Envisat/MIPAS, Odin/SMR, Aura/MLS, Envisat/SCIAMACHY and SCISAT/ACE-FTS it is further investigated if there is a decrease in temperature and/or increase of water vapour (H2O) observed in the polar regions similar to that observed at midlatitudes and in the tropics. Performing linear regression analyses we derive from the Envisat/MIPAS (2002-2012) and Aura/MLS (2004-2014) observations predominantly positive changes in the potential temperature range 350 to 1000 K. The linear changes in water vapour derived from Envisat/MIPAS observations are largely insignificant, while those from Aura/MLS are mostly significant. For the temperature neither of the two instruments indicate any significant changes. Given the strong inter-annual variation observed in water vapour and particular temperature the severe denitrification observed in 2010/11 cannot be directly related to any changes in water vapour and temperature since the millennium. However, the observations indicate a clear correlation between cold winters and enhanced water vapour mixing ratios. This indicates a connection between dynamical and radiative processes that govern water vapour and temperature in the Arctic lower stratosphere.
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| 6. |
- Kim, S. W., et al.
(författare)
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Evaluations of NOx and highly reactive VOC emission inventories in Texas and their implications for ozone plume simulations during the Texas Air Quality Study 2006
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:22, s. 11361-11386
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Tidskriftsartikel (refereegranskat)abstract
- Satellite and aircraft observations made during the 2006 Texas Air Quality Study (TexAQS) detected strong urban, industrial and power plant plumes in Texas. We simulated these plumes using the Weather Research and Forecasting-Chemistry (WRF-Chem) model with input from the US EPA's 2005 National Emission Inventory (NEI-2005), in order to evaluate emissions of nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs) in the cities of Houston and Dallas-FortWorth. We compared the model results with satellite retrievals of tropospheric nitrogen dioxide (NO2) columns and airborne in-situ observations of several trace gases including NOx and a number of VOCs. The model and satellite NO2 columns agree well for regions with large power plants and for urban areas that are dominated by mobile sources, such as Dallas. How-ever, in Houston, where significant mobile, industrial, and inport marine vessel sources contribute to NOx emissions, the model NO2 columns are approximately 50 %-70 % higher than the satellite columns. Similar conclusions are drawn from comparisons of the model results with the TexAQS 2006 aircraft observations in Dallas and Houston. For Dallas plumes, the model-simulated NO2 showed good agreement with the aircraft observations. In contrast, the model-simulated NO2 is similar to 60 % higher than the aircraft observations in the Houston plumes. Further analysis indicates that the NEI-2005 NOx emissions over the Houston Ship Channel area are overestimated while the urban Houston NOx emissions are reasonably represented. The comparisons of model and aircraft observations confirm that highly reactive VOC emissions originating from industrial sources in Houston are underestimated in NEI-2005. The update of VOC emissions based on Solar Occultation Flux measurements during the field campaign leads to improved model simulations of ethylene, propylene, and formaldehyde. Reducing NOx emissions in the Houston Ship Channel and increasing highly reactive VOC emissions from the point sources in Houston improve the model's capability of simulating ozone (O-3) plumes observed by the NOAA WP-3D aircraft, although the deficiencies in the model O-3 simulations indicate that many challenges remain for a full understanding of the O-3 formation mechanisms in Houston.
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| 7. |
- Spolaor, A., et al.
(författare)
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Seasonality of halogen deposition in polar snow and ice
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14, s. 9613-9622
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Tidskriftsartikel (refereegranskat)abstract
- The atmospheric chemistry of iodine and bromine in Polar regions is of interest due to the key role of halogens in many atmospheric processes, particularly tropospheric ozone destruction. Bromine is emitted from the open ocean but is enriched above first-year sea ice during springtime bromine explosion events, whereas iodine emission is at- tributed to biological communities in the open ocean and hosted by sea ice. It has been previously demonstrated that bromine and iodine are present in Antarctic ice over glacial– interglacial cycles. Here we investigate seasonal variability of bromine and iodine in polar snow and ice, to evaluate their emission, transport and deposition in Antarctica and the Arc- tic and better understand potential links to sea ice. We find that bromine and iodine concentrations and Br enrichment (relative to sea salt content) in polar ice do vary seasonally in Arctic snow and Antarctic ice. Although seasonal vari- ability in halogen emission sources is recorded by satellite- based observations of tropospheric halogen concentrations, seasonal patterns observed in snowpack are likely also in- fluenced by photolysis-driven processes. Peaks of bromine concentration and Br enrichment in Arctic snow and Antarc- tic ice occur in spring and summer, when sunlight is present. A secondary bromine peak, observed at the end of summer, is attributed to bromine deposition at the end of the polar day. Iodine concentrations are largest in winter Antarctic ice strata, contrary to contemporary observations of summer maxima in iodine emissions. These findings support previous observations of iodine peaks in winter snow strata attributed to the absence of sunlight-driven photolytic re-mobilisation of iodine from surface snow. Further investigation is required to confirm these proposed mechanisms explaining observa- tions of halogens in polar snow and ice, and to evaluate the extent to which halogens may be applied as sea ice proxies.
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