| 241. |
- Khosrawi, Farahnaz, et al.
(författare)
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Denitrification and polar stratospheric cloud formation during the Arctic winter 2009/2010
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:16, s. 8471-8487
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Tidskriftsartikel (refereegranskat)abstract
- The sedimentation of HNO3 containing PolarStratospheric Cloud (PSC) particles leads to a permanent re-moval of HNO3 and thus to a denitrification of the strato-sphere, an effect which plays an important role in strato-spheric ozone depletion. The polar vortex in the Arctic win-ter 2009/2010 was very cold and stable between end of De-cember and end of January. Strong denitrification between 475 to 525 K was observed in the Arctic in mid of Januaryby the Odin Sub Millimetre Radiometer (Odin/SMR). Thiswas the strongest denitrification that had been observed inthe entire Odin/SMR measuring period (2001–2010). Lidarmeasurements of PSCs were performed in the area of Kiruna,Northern Sweden with the IRF (Institutet för Rymdfysik) li-odar and with the Esrange lidar in January 2010. The measurements show that PSCs were present over the area of Kirunaduring the entire period of observations. The formation ofPSCs during the Arctic winter 2009/2010 is investigated using a microphysical box model. Box model simulationsare performed along air parcel trajectories calculated sixdays backward according to the PSC measurements with the ground-based lidar in the Kiruna area. From the temperaturehistory of the backward trajectories and the box model simulations we find two PSC regions, one over Kiruna accordingto the measurements made in Kiruna and one north of Scandinavia which is much colder, reaching also temperatures below Tice. Using the box model trajectories together with the observations of Odin/SMR,Aura/MLS (Microwave Limb Sounder), CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations)and the ground-based lidar we investigate how and by whichtype of PSC particles the denitrification that was observedduring the Arctic winter 2009/2010 was caused. From ouranalysis we find that due to an unusually strong synopticcooling event in mid January, ice particle formation on NATmay be a possible formation mechanism during that particu-lar winter that may have caused the denitrification observed in mid January. In contrast, the denitrification that was observed in the beginning of January could have been caused by the sedimentation of NAT particles that formed on moun-tain wave ice clouds.
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| 242. |
- Khosrawi, Farahnaz, 1971-, et al.
(författare)
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Evaluation of CLaMS, KASIMA and ECHAM5/MESSy1 simulations in the lower stratosphere using observations of Odin/SMR and ILAS/ILAS-II
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:15, s. 5759-5783
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Tidskriftsartikel (refereegranskat)abstract
- 1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one solar occultation data set derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one limb sounding data set derived from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppbv, thus in air masses of tropical character. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.
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| 243. |
- Khosrawi, Farahnaz, et al.
(författare)
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Particle formation in the Arctic free troposphere during the ASTAR 2004 campaign: A case study on the influence of vertical motion on the binary homogeneous nucleation of H2SO4/H2O
- 2010
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10, s. 1105-1120
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Tidskriftsartikel (refereegranskat)abstract
- During the ASTAR (Arctic Study of Tropospheric Aerosol and Radiation) campaign nucleation mode particles (4 to 13 nm) were quite frequently observed at altitudes below 4000 m. However, in the upper free troposphere, nucleation mode particles were only observed once, namely during the flight on 24 May 2004 (7000 m). To investigate if vertical motion are the reason for this difference that on one particular day nucleation mode particles were observed but not on the other days we employ a microphysical box model. The box model simulations were performed along air parcel trajectories calculated 6-d backwards based on European Center for Medium-Range Weather Forecasts (ECMWF) meteorological analyses using state parameters such as pressure and temperature in combination with additional parameters such as vertical stability. Box model simulations were performed for the 24 May where nucleation mode particles were observed (nucleation event) as well as for the day with measurements before and after (22 and 26 May) which are representative for no nucleation (none nucleation event). A nucleation burst was simulated along all trajectories, however, in the majority of the simulations the nucleation rate was either too low or too high so that no nucleation mode particles were left at the time were the measurements were performed. Further, the simulation results could be divided into three cases. Thereby, we found that for case 1 the temperature was the only driving mechanism while for case 2 and 3 vertical motion have influenced the formation of new particles. The reason why nucleation mode particles were observed on 24 May, but not on the other day, can be explained by the conditions under which particle formation occurred. On 24 May the particle formation was caused by a slow updraft, while on the other two days the particle formation was caused by a fast updraft.
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| 244. |
- 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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| 245. |
- Kiefer, M., et al.
(författare)
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Characterization of MIPAS elevation pointing
- 2007
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 7:6, s. 1615-1628
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Tidskriftsartikel (refereegranskat)abstract
- Sufficient knowledge of the pointing is essential for analyses of limb emission measurements. The scientific retrieval processor for MIPAS on ENVISAT operated at IMK allows the retrieval of pointing information in terms of tangent altitudes along with temperature. The retrieved tangent altitudes are independent of systematic offsets in the engineering Line-Of-Sight (LOS) information delivered with the ESA Level 1b product. The difference of pointing retrieved from the reprocessed high resolution MIPAS spectra and the engineering pointing information was examined with respect to spatial/temporal behaviour. Among others the following characteristics of MIPAS pointing could be identified: Generally the engineering tangent altitudes are too high by 0–1.8 km with conspicuous variations in this range over time. Prior to December of 2003 there was a drift of about 50–100 m/h, which was due to a slow change in the satellite attitude. A correction of this attitude is done twice a day, which leads to discontinuities in the order of 1–1.5 km in the tangent altitudes. Occasionally discontinuities up to 2.5 km are found, as already reported from MIPAS and SCIAMACHY observations. After an update of the orbit position software in December 2003 values of drift and jumps are much reduced. There is a systematic difference in the mispointing between the poles which amounts to 1.5–2 km, i.e. there is a conspicuous orbit-periodic feature. The analysis of the correlation between the instrument's viewing angle azimuth and differential mispointing supports the hypotheses that a major part of this latter phenomenon can be attributed to an error in the roll angle of the satellite/instrument system of approximately 42 mdeg. One conclusion is that ESA level 2 data should be compared to other data exclusively on tangent pressure levels. Complementary to IMK data, ESA operational LOS calibration results were used to characterize MIPAS pointing. For this purpose MIPAS is used as a radiometer while the passage of infrared bright stars through the instrument's field of view is recorded. Deviation from expected time of passage gives information about mispointing. Results are: a pronounced seasonal variation of the LOS is seen before a correction of on-board software took place in December of 2003. Further a pitch bias of 26 mdeg with respect to the platform attitude information is found, which corresponds to 1.45 km tangent altitude offset towards low altitudes.
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| 246. |
- Kim, J., et al.
(författare)
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Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:1, s. 293-304
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Tidskriftsartikel (refereegranskat)abstract
- Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study,we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at sub-saturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from alpha-pinene oxidation. The hygroscopicity parameter kappa decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 x 10(6) molecules cm(-3) in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured kappa of 15 nm particles was 0.31 +/- 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (kappa(DMAS) similar to 0.28). Furthermore, the difference in kappa between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The kappa values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from alpha-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
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| 247. |
- 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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| 248. |
- Kirillova, Elena, et al.
(författare)
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Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:3, s. 1413-1422
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Tidskriftsartikel (refereegranskat)abstract
- High loadings of anthropogenic carbonaceous aerosols in Chinese air influence the air quality for over one billion people and impact the regional climate. A large fraction (17-80 %) of this aerosol carbon is water-soluble, promoting cloud formation and thus climate cooling. Recent findings, however, suggest that water-soluble carbonaceous aerosols also absorb sunlight, bringing additional direct and indirect climate warming effects, yet the extent and nature of light absorption by this water-soluble brown carbon and its relation to sources is poorly understood. Here, we combine source estimates constrained by dual carbon isotopes with light-absorption measurements of water-soluble organic carbon (WSOC) for a March 2011 campaign at the Korea Climate Observatory at Gosan (KCOG), a receptor station in SE Yellow Sea for the outflow from northern China. The mass absorption cross section at 365 nm (MAC(365)) of WSOC for air masses from N. China were in general higher (0.8-1.1 m(2) g(-1)), than from other source regions (0.3-0.8 m(2) g(-1)). However, this effect corresponds to only 2-10% of the radiative forcing caused by light absorption by elemental carbon. Radiocarbon constraints show that the WSOC in Chinese outflow had significantly higher fraction fossil sources (30-50 %) compared to previous findings in S. Asia, N. America and Europe. Stable carbon (delta C-13) measurements were consistent with aging during long-range air mass transport for this large fraction of carbonaceous aerosols.
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| 249. |
- Kirkwood, Sheila, et al.
(författare)
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Turbulence associated with mountain waves over Northern Scandinavia : a case study using the ESRAD VHF radar and the WRF mesoscale model
- 2010
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10, s. 3583-3599
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Tidskriftsartikel (refereegranskat)abstract
- We use measurements by the 52 MHz wind-profiling radar ESRAD, situated near Kiruna in Arctic Sweden, and simulations using the Advanced Research and Weather Forecasting model, WRF, to study vertical winds and turbulence in the troposphere in mountain-wave conditions on 23, 24 and 25 January 2003. We find that WRF can accurately match the vertical wind signatures at the radar site when the spatial resolution for the simulations is 1 km. The horizontal and vertical wavelengths of the dominating mountain-waves are ~10–20 km and the amplitudes in vertical wind 1–2 m/s. Turbulence below 5500 m height, is seen by ESRAD about 40% of the time. This is a much higher rate than WRF predictions for conditions of Richardson number (Ri) <1 but similar to WRF predictions of Ri<2. WRF predicts that air crossing the 100 km wide model domain centred on ESRAD has a ~10% chance of encountering convective instabilities (Ri<0) somewhere along the path. The cause of low Ri is a combination of wind-shear at synoptic upper-level fronts and perturbations in static stability due to the mountain-waves. Comparison with radiosondes suggests that WRF underestimates wind-shear and the occurrence of thin layers with very low static stability, so that vertical mixing by turbulence associated with mountain waves may be significantly more than suggested by the model
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| 250. |
- Kivekäs, Niku, et al.
(författare)
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Contribution of ship traffic to aerosol particle concentrations downwind of a major shipping lane
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:16, s. 8255-8267
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Tidskriftsartikel (refereegranskat)abstract
- Particles in the atmosphere are of concern due to their toxic properties and effects on climate. In coastal areas, ship emissions can be a significant anthropogenic source. In this study we investigated the contribution from ship emissions to the total particle number and mass concentrations at a remote location. We studied the particle number concentration (12 to 490 nm in diameter), the mass concentration (12 to 150 nm in diameter) and number and volume size distribution of aerosol particles in ship plumes for a period of 4.5 months at Hovsore, a coastal site on the western coast of Jutland in Denmark. During episodes of western winds, the site is about 50 km downwind of a major shipping lane and the plumes are approximately 1 hour old when they arrive at the site. We have used a sliding percentile-based method for separating the plumes from the measured background values and to calculate the ship plume contribution to the total particle number and PM0.15 mass concentration (mass of particles below 150 nm in diameter, converted from volume assuming sphericity) at the site. The method is not limited to particle number or volume concentration, but can also be used for different chemical species in both particle and gas phase. The total number of analyzed ship plumes was 726, covering on average 19% of the time when air masses were arriving at the site over the shipping lane. During the periods when plumes were present, the particle concentration exceeded the background values on average by 790 cm(-3) by number and 0.10 gm(-3) by mass. The corresponding daily average values were 170 cm-3 and 0.023 gm-3, respectively. This means that the ship plumes contributed between 11 and 19% to the particle number concentration and between 9 and 18% to PM0.15 during days when air was arriving over the shipping lane. The estimated annual contribution from ship plumes, where all wind directions were included, was in the range of 5-8% in particle number concentration and 4-8% in PM0.15.
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