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Sökning: L773:1680 7316 > Mellqvist Johan 1965 > Chalmers tekniska högskola

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  • Angelbratt, Jon, 1981-, et al. (författare)
  • A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network
  • 2011
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 11:13, s. 6167-6183
  • Tidskriftsartikel (refereegranskat)abstract
    • Total columns measured with the ground-based solar FTIR technique are highly variable in time due to atmospheric chemistry and dynamics in the atmosphere above the measurement station. In this paper, a multiple regression model with anomalies of air pressure, total columns of hydrogen fluoride (HF) and carbon monoxide (CO) and tropopause height are used to reduce the variability in the methane (CH(4)) and nitrous oxide (N(2)O) total columns to estimate reliable linear trends with as small uncertainties as possible. The method is developed at the Harestua station (60 degrees N, 11 degrees E, 600 ma.s.l.) and used on three other European FTIR stations, i.e. Jungfraujoch (47 degrees N, 8 degrees E, 3600 ma.s.l.), Zugspitze (47 degrees N, 11 degrees E, 3000 ma.s.l.), and Kiruna (68 degrees N, 20 degrees E, 400 ma.s.l.). Linear CH(4) trends between 0.13 +/- 0.01-0.25 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2009 period. A piecewise model with three separate linear trends, connected at change points, was used to estimate the short term fluctuations in the CH(4) total columns. This model shows a growth in 1996-1999 followed by a period of steady state until 2007. From 2007 until 2009 the atmospheric CH(4) amount increases between 0.57 +/- 0.22-1.15 +/- 0.17% yr(-1). Linear N(2)O trends between 0.19 +/- 0.01-0.40 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2007 period, here with the strongest trend at Harestua and Kiruna and the lowest at the Alp stations. From the N(2)O total columns crude tropospheric and stratospheric partial columns were derived, indicating that the observed difference in the N(2)O trends between the FTIR sites is of stratospheric origin. This agrees well with the N(2)O measurements by the SMR instrument onboard the Odin satellite showing the highest trends at Harestua, 0.98 +/- 0.28% yr(-1), and considerably smaller trends at lower latitudes, 0.27 +/- 0.25% yr(-1). The multiple regression model was compared with two other trend methods, the ordinary linear regression and a Bootstrap algorithm. The multiple regression model estimated CH(4) and N(2)O trends that differed up to 31% compared to the other two methods and had uncertainties that were up to 300% lower. Since the multiple regression method were carefully validated this stresses the importance to account for variability in the total columns when estimating trend from solar FTIR data.
  • Angelbratt, Jon, 1981-, et al. (författare)
  • Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model
  • 2011
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 11:17, s. 9253-9269
  • Tidskriftsartikel (refereegranskat)abstract
    • Trends in the CO and C(2)H(6) partial columns (similar to 0-15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to -0.45 +/- 0.16%yr(-1), -1.00 +/- 0.24%yr(-1), -0.62 +/- 0.19%yr(-1) and -0.61 +/- 0.16%yr(-1), respectively. The corresponding trends for C(2)H(6) are -1.51 +/- 0.23%yr(-1), -2.11 +/- 0.30%yr(-1), -1.09 +/- 0.25%yr(-1) and -1.14 +/- 0.18%yr(-1). All trends are presented with their 2-sigma confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH(4) and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C(2)H(6) partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Alesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22% deviation for CO and 14-31% deviation for C(2)H(6). Their seasonal amplitude is captured within 6-35% and 9-124% for CO and C(2)H(6), respectively. However, 61-98% of the CO and C(2)H(6) partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9% and 37-50% of the measurements for CO and C(2)H(6), respectively. The global model sensitivity for assumptions made in this paper is also analyzed.
  • de Foy, B., et al. (författare)
  • Modelling constraints on the emission inventory and on vertical dispersion for CO and SO2 in the Mexico City Metropolitan Area using Solar FTIR and zenith sky UV spectroscopy
  • 2007
  • Ingår i: Atmospheric Chemistry And Physics. - 1680-7316. ; 7, s. 781-801
  • Tidskriftsartikel (refereegranskat)abstract
    • Emissions of air pollutants in and around urban areas lead to negative health impacts on the population. To estimate these impacts, it is important to know the sources and transport mechanisms of the pollutants accurately. Mexico City has a large urban fleet in a topographically constrained basin leading to high levels of carbon monoxide ( CO). Large point sources of sulfur dioxide (SO2) surrounding the basin lead to episodes with high concentrations. An Eulerian grid model (CAMx) and a particle trajectory model ( FLEXPART) are used to evaluate the estimates of CO and SO2 in the current emission inventory using mesoscale meteorological simulations from MM5. Vertical column measurements of CO are used to constrain the total amount of emitted CO in the model and to identify the most appropriate vertical dispersion scheme. Zenith sky UV spectroscopy is used to estimate the emissions of SO2 from a large power plant and the Popocatepetl volcano. Results suggest that the models are able to identify correctly large point sources and that both the power plant and the volcano impact the MCMA. Modelled concentrations of CO based on the current emission inventory match observations suggesting that the current total emissions estimate is correct. Possible adjustments to the spatial and temporal distribution can be inferred from model results. Accurate source and dispersion modelling provides feedback for development of the emission inventory, verification of transport processes in air quality models and guidance for policy decisions.
  • Gardiner, T., et al. (författare)
  • Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments
  • 2008
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 8:22, s. 6719-6727
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper describes the statistical analysis of annual trends in long term datasets of greenhouse gas measurements taken over ten or more years. The analysis technique employs a bootstrap resampling method to determine both the long-term and intra-annual variability of the datasets, together with the uncertainties on the trend values. The method has been applied to data from a European network of ground-based solar FTIR instruments to determine the trends in the tropospheric, stratospheric and total columns of ozone, nitrous oxide, carbon monoxide, methane, ethane and HCFC-22. The suitability of the method has been demonstrated through statistical validation of the technique, and comparison with ground-based in-situ measurements and 3-D atmospheric models.
  • Hopfner, M., et al. (författare)
  • Validation of MIPAS ClONO2 measurements
  • 2007
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 7, s. 257-281
  • Tidskriftsartikel (refereegranskat)abstract
    • Altitude profiles of ClONO2 retrieved with the IMK (Institut fur Meteorologie und Klimaforschung) science-oriented data processor from MIPAS/Envisat (Michelson Interferometer for Passive Atmospheric Sounding on Envisat) mid-infrared limb emission measurements between July 2002 and March 2004 have been validated by comparison with balloon-borne (Mark IV, FIRS2, MIPAS-B), airborne (MIPAS-STR), ground-based (Spitsbergen, Thule, Kiruna, Harestua, Jungfraujoch, Izana, Wollongong, Lauder), and spaceborne (ACE-FTS) observations. With few exceptions we found very good agreement between these instruments and MIPAS with no evidence for any bias in most cases and altitude regions. For balloon-borne measurements typical absolute mean differences are below 0.05 ppbv over the whole altitude range from 10 to 39 km. In case of ACE-FTS observations mean differences are below 0.03 ppbv for observations below 26 km. Above this altitude the comparison with ACE-FTS is affected by the photochemically induced diurnal variation of ClONO2. Correction for this by use of a chemical transport model led to an overcompensation of the photochemical effect by up to 0.1 ppbv at altitudes of 30-35 km in case of MIPAS-ACE-FTS comparisons while for the balloon-borne observations no such inconsistency has been detected. The comparison of MIPAS derived total column amounts with ground-based observations revealed no significant bias in the MIPAS data. Mean differences between MIPAS and FTIR column abundances are 0.11 +/- 0.12 x 10(14) cm(-2) (1.0 +/- 1.1%) and -0.09 +/- 0.19 x 10(14) cm(-2) (-0.8 +/- 1.7%), depending on the coincidence criterion applied. chi(2) tests have been performed to assess the combined precision estimates of MIPAS and the related instruments. When no exact coincidences were available as in case of MIPAS-FTIR or MIPAS-ACE-FTS comparisons it has been necessary to take into consideration a coincidence error term to account for chi(2) deviations. From the resulting chi(2) profiles there is no evidence for a systematic over/underestimation of the MIPAS random error analysis.
  • Kim, S. W., et al. (författare)
  • 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
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 11:22, s. 11361-11386
  • 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.
  • Liu, L., et al. (författare)
  • Photochemical modelling in the Po basin with focus on formaldehyde and ozone
  • 2007
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 7, s. 121-137
  • Tidskriftsartikel (refereegranskat)abstract
    • As part of the EU project FORMAT ( Formaldehyde as a Tracer of Oxidation in the Troposphere), a field campaign was carried out in the vicinity of Milan during the summer of 2002. Results from a 3-D regional chemical transport model (NILU RCTM) were used to interpret the observations focusing primarily on HCHO and ozone. The performance of the model was assessed by comparing model results with ground based and aircraft measurements. The model results show good agreement with surface measurements, and the model is able to reproduce the photochemical episodes during fair weather days. The comparison indicates that the model can represent well the HCHO concentrations as well as their temporal and spatial variability. The relationship between HCHO and (O-3 x H2O) was used to validate the model ability to predict the HCHO concentrations. Further analysis revealed the importance of the representativeness of different instruments: in-situ concentrations might be locally enhanced by emissions, while long path measurements over a forest can be influenced by rapid formation of HCHO from isoprene. The model is able to capture the plume from the city of Milan and the modelled levels agree generally well with the aircraft measurements, although the wind fields used in the model can lead to a displacement of the ozone plume. During the campaign period, O3 levels were seldom higher than 80 ppb, the peak surface ozone maxima reached 90 ppb. Those relatively low values can be explained by low emissions during the August vacation and unstable weather conditions in this period. The modelled Delta O-3/Delta NOz slope at Alzate of 5.1 agrees well with the measured slope of 4.9.
  • Parrish, D. D., et al. (författare)
  • Primary and secondary sources of formaldehyde in urban atmospheres: Houston Texas region
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 12:7, s. 3273-3288
  • Tidskriftsartikel (refereegranskat)abstract
    • We evaluate the rates of secondary production and primary emission of formaldehyde (CH2O) from petrochemical industrial facilities and on-road vehicles in the Houston Texas region. This evaluation is based upon ambient measurements collected during field studies in 2000, 2006 and 2009. The predominant CH2O source (92 +/- 4% of total) is secondary production formed during the atmospheric oxidation of highly reactive volatile organic compounds (HRVOCs) emitted from the petrochemical facilities. Smaller contributions are primary emissions from these facilities (4 +/- 2%), and secondary production (similar to 3%) and primary emissions (similar to 1%) from vehicles. The primary emissions from both sectors are well quantified by current emission inventories. Since secondary production dominates, control efforts directed at primary CH2O emissions cannot address the large majority of CH2O sources in the Houston area, although there may still be a role for such efforts. Ongoing efforts to control alkene emissions from the petrochemical facilities, as well as volatile organic compound emissions from the motor vehicle fleet, will effectively reduce the CH2O concentrations in the Houston region. We do not address other emission sectors, such as off-road mobile sources or secondary formation from biogenic hydrocarbons. Previous analyses based on correlations between ambient concentrations of CH2O and various marker species have suggested much larger primary emissions of CH2O, but those results neglect confounding effects of dilution and loss processes, and do not demonstrate the causes of the observed correlations. Similar problems must be suspected in any source apportionment analysis of secondary species based upon correlations of ambient concentrations of pollutants.
  • Strong, K., et al. (författare)
  • Validation of ACE-FTS N2O measurements
  • 2008
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 8, s. 4759-4786
  • Tidskriftsartikel (refereegranskat)abstract
    • The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within ±10 ppbv. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within ±5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.
  • Vigouroux, C., et al. (författare)
  • Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations
  • 2008
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 8, s. 6865-6886
  • Tidskriftsartikel (refereegranskat)abstract
    • Within the European project UFTIR (Time series of Upper Free Troposphere observations from an European ground-based FTIR network), six ground-based stations in Western Europe, from 79 degrees N to 28 degrees N, all equipped with Fourier Transform infrared (FTIR) instruments and part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to evaluate the trends of several direct and indirect greenhouse gases over the period 1995-2004. The retrievals of CO, CH4, C2H6, N2O, CHClF2, and O-3 have been optimized. Using the optimal estimation method, some vertical information can be obtained in addition to total column amounts. A bootstrap resampling method has been implemented to determine annual partial and total column trends for the target gases. The present work focuses on the ozone results. The retrieved time series of partial and total ozone columns are validated with ground-based correlative data (Brewer, Dobson, UV-Vis, ozonesondes, and Lidar). The observed total column ozone trends are in agreement with previous studies: 1) no total column ozone trend is seen at the lowest latitude station Izana (28 degrees N); 2) slightly positive total column trends are seen at the two mid-latitude stations Zugspitze and Jungfraujoch (47 degrees N), only one of them being significant; 3) the highest latitude stations Harestua (60 degrees N), Kiruna (68 degrees N) and Ny-Alesund (79 degrees N) show significant positive total column trends. Following the vertical information contained in the ozone FTIR retrievals, we provide partial columns trends for the layers: ground-10 km, 10-18 km, 18-27 km, and 27-42 km, which helps to distinguish the contributions from dynamical and chemical changes on the total column ozone trends. We obtain no statistically significant trends in the ground-10 km layer for five out of the six ground-based stations. We find significant positive trends for the lower-most stratosphere at the two mid-latitude stations, and at Ny-Alesund. We find smaller, but significant trends for the 18 27 km layer at Kiruna, Harestua, Jungfraujoch, and Izana. The results for the upper layer are quite contrasted: we find significant positive trends at Kiruna, Harestua, and Jungfraujoch, and significant negative trends at Zugspitze and Izana. These ozone partial columns trends are discussed and compared with previous studies.
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