scholarly journals Global carbonyl sulfide (OCS) measured by MIPAS/Envisat during 2002–2012

2016 ◽  
Author(s):  
Norbert Glatthor ◽  
Michael Höpfner ◽  
Adrian Leyser ◽  
Gabriele P. Stiller ◽  
Thomas von Clarmann ◽  
...  

Abstract. We present a global OCS data set covering the period June 2002 to April 2012, derived from FTIR limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite. The vertical resolution is 4–5 km in the height region 6–15 km and 15 km at 40 km altitude. The total estimated error amounts to 40–50 pptv between 10 and 20 km and to 120 pptv at 40 km altitude. MIPAS OCS data show no systematic bias with respect to balloon observations, with deviations mostly below ±50 pptv. However, they are systematically higher than the OCS volume mixing ratios of the ACE-FTS instrument on SCISAT, with maximum deviations of up to 100 pptv in the altitude region 13–16 km. The data set of MIPAS OCS exhibits only moderate interannual variations and low interhemispheric differences. Average concentrations at 10 km altitude range from 480 pptv at high latitudes to 500–510 pptv in the tropics and at northern mid-latitudes. Seasonal variations at 10 km altitude amount up to 35 pptv in the northern and up to 15 pptv in the southern hemisphere. Northern hemispheric OCS abundances at 10 km altitude peak in June in the tropics and around October at high latitudes, while the respective southern hemispheric maxima were observed in July and in November. Global OCS distributions at 250 hPa (~ 10–11 km) show enhanced values at low latitudes, peaking during boreal summer above the western Pacific and the Indian Ocean, which indicates oceanic release. Further, a region of depleted OCS amounts extending from Brazil to central and southern Africa was detected at this altitude, which is most pronounced in austral summer. This depletion is related to seasonally varying vegetative uptake by the tropical forests. Typical signatures of biomass burning like the southern hemispheric biomass burning plume are not visible in MIPAS data, indicating that this process is only a minor source of tropospheric OCS. At the 150 hPa level (~ 13–14 km) enhanced amounts of OCS were also observed inside the Asian Monsoon Anticyclone, but this enhancement is not especially outstanding as compared to other low latitude regions at the same altitude. At the 80 hPa level (~ 17–18 km) equatorward transport of mid-latitude air masses containing lower OCS amounts around the summertime anticyclones was observed. A significant trend could not be detected in tropospheric MIPAS OCS amounts, which points to globally balanced sources and sinks.

2017 ◽  
Vol 17 (4) ◽  
pp. 2631-2652 ◽  
Author(s):  
Norbert Glatthor ◽  
Michael Höpfner ◽  
Adrian Leyser ◽  
Gabriele P. Stiller ◽  
Thomas von Clarmann ◽  
...  

Abstract. We present a global carbonyl sulfide (OCS) data set covering the period June 2002 to April 2012, derived from FTIR (Fourier transform infrared) limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite. The vertical resolution is 4–5 km in the height region 6–15 km and 15 at 40 km altitude. The total estimated error amounts to 40–50 pptv between 10 and 20 km and to 120 pptv at 40 km altitude. MIPAS OCS data show no systematic bias with respect to balloon observations, with deviations mostly below ±50 pptv. However, they are systematically higher than the OCS volume mixing ratios of the ACE-FTS instrument on SCISAT, with maximum deviations of up to 100 pptv in the altitude region 13–16 km. The data set of MIPAS OCS exhibits only moderate interannual variations and low interhemispheric differences. Average concentrations at 10 km altitude range from 480 pptv at high latitudes to 500–510 pptv in the tropics and at northern mid-latitudes. Seasonal variations at 10 km altitude amount to up to 35 pptv in the Northern and up to 15 pptv in the Southern Hemisphere. Northern hemispheric OCS abundances at 10 km altitude peak in June in the tropics and around October at high latitudes, while the respective southern hemispheric maxima were observed in July and in November. Global OCS distributions at 250 hPa (∼ 10–11 km) show enhanced values at low latitudes, peaking during boreal summer above the western Pacific and the Indian Ocean, which indicates oceanic release. Further, a region of depleted OCS amounts extending from Brazil to central and southern Africa was detected at this altitude, which is most pronounced in austral summer. This depletion is related to seasonally varying vegetative uptake by the tropical forests. Typical signatures of biomass burning like the southern hemispheric biomass burning plume are not visible in MIPAS data, indicating that this process is only a minor source of upper tropospheric OCS. At the 150 hPa level (∼ 13–14 km) enhanced amounts of OCS were also observed inside the Asian monsoon anticyclone, but this enhancement is not especially outstanding compared to other low latitude regions at the same altitude. At the 80 hPa level (∼ 17–18 km), equatorward transport of mid-latitude air masses containing lower OCS amounts around the summertime anticyclones was observed. A significant trend could not be detected in upper tropospheric MIPAS OCS amounts, which points to globally balanced sources and sinks. Simulations with the ECHAM-MESSy model reproduce the observed latitudinal cross sections fairly well.


2014 ◽  
Vol 142 (4) ◽  
pp. 1556-1569 ◽  
Author(s):  
Hongyan Zhu ◽  
Matthew C. Wheeler ◽  
Adam H. Sobel ◽  
Debra Hudson

Abstract The skill with which a coupled ocean–atmosphere model is able to predict precipitation over a range of time scales (days to months) is analyzed. For a fair comparison across the seamless range of scales, the verification is performed using data averaged over time windows equal in length to the lead time. At a lead time of 1 day, skill is greatest in the extratropics around 40°–60° latitude and lowest around 20°, and has a secondary local maximum close to the equator. The extratropical skill at this short range is highest in the winter hemisphere, presumably due to the higher predictability of winter baroclinic systems. The local equatorial maximum comes mostly from the Pacific Ocean, and thus appears to be mostly from El Niño–Southern Oscillation (ENSO). As both the lead time and averaging window are simultaneously increased, the extratropical skill drops rapidly with lead time, while the equatorial maximum remains approximately constant, causing the equatorial skill to exceed the extratropical at leads of greater than 4 days in austral summer and 1 week in boreal summer. At leads longer than 2 weeks, the extratropical skill flattens out or increases, but remains below the equatorial values. Comparisons with persistence confirm that the model beats persistence for most leads and latitudes, including for the equatorial Pacific where persistence is high. The results are consistent with the view that extratropical predictability is mostly derived from synoptic-scale atmospheric dynamics, while tropical predictability is primarily derived from the response of moist convection to slowly varying forcing such as from ENSO.


2011 ◽  
Vol 11 (13) ◽  
pp. 6701-6719 ◽  
Author(s):  
H. Yashiro ◽  
K. Sudo ◽  
S. Yonemura ◽  
M. Takigawa

Abstract. The global tropospheric distribution of molecular hydrogen (H2) and its uptake by the soil are simulated using a model called CHemical AGCM (atmospheric general circulation model) for the Study of the Environment and Radiative forcing (CHASER), which incorporates a two-layered soil diffusion/uptake process component. The simulated distribution of deposition velocity over land is influenced by regional climate, and has a global average of 3.3×10−2 cm s−1. In the region north of 30° N, the amount of soil uptake shows a large seasonal variation corresponding to change in biological activity due to soil temperature and change in diffusion suppression by snow cover. In the temperate and humid regions in the mid- to low- latitudes, the uptake is mostly influenced by the soil air ratio, which controls the gas diffusivity in the soil. In the semi-arid regions, water stress and high temperatures contribute to the reduction of biological activity, as well as to the seasonal variation in the deposition velocity. A comparison with the observations shows that the model reproduces both the distribution and seasonal variation of H2 relatively well. The global burden and tropospheric lifetime of H2 are 150 Tg and 2.0 yr, respectively. The seasonal variation in H2 mixing ratios at the northern high latitudes is mainly controlled by a large seasonal change in the soil uptake. In the Southern Hemisphere, seasonal change in net chemical production and inter-hemispheric transport are the dominant causes of the seasonal cycle, while large biomass burning contributes significantly to the seasonal variation in the tropics and subtropics. Both observations and the model show large inter-annual variations, especially for the period 1997–1998, associated with large biomass burning in the tropics and at Northern Hemisphere high latitudes. The soil uptake shows relatively small inter-annual variability compared with the biomass burning signal. Given that the thickness of biologically inactive layer plays an important role in the soil uptake of H2, its value in the model is chosen to achieve agreement with the observed H2 trends. Uncertainty of the estimated soil uptake flux in the semi-arid region is still large, reflecting the discrepancy in the observed and modeled seasonal variations.


2014 ◽  
Vol 14 (12) ◽  
pp. 6177-6194 ◽  
Author(s):  
R. L. Thompson ◽  
K. Ishijima ◽  
E. Saikawa ◽  
M. Corazza ◽  
U. Karstens ◽  
...  

Abstract. This study examines N2O emission estimates from five different atmospheric inversion frameworks based on chemistry transport models (CTMs). The five frameworks differ in the choice of CTM, meteorological data, prior uncertainties and inversion method but use the same prior emissions and observation data set. The posterior modelled atmospheric N2O mole fractions are compared to observations to assess the performance of the inversions and to help diagnose problems in the modelled transport. Additionally, the mean emissions for 2006 to 2008 are compared in terms of the spatial distribution and seasonality. Overall, there is a good agreement among the inversions for the mean global total emission, which ranges from 16.1 to 18.7 TgN yr−1 and is consistent with previous estimates. Ocean emissions represent between 31 and 38% of the global total compared to widely varying previous estimates of 24 to 38%. Emissions from the northern mid- to high latitudes are likely to be more important, with a consistent shift in emissions from the tropics and subtropics to the mid- to high latitudes in the Northern Hemisphere; the emission ratio for 0–30° N to 30–90° N ranges from 1.5 to 1.9 compared with 2.9 to 3.0 in previous estimates. The largest discrepancies across inversions are seen for the regions of South and East Asia and for tropical and South America owing to the poor observational constraint for these areas and to considerable differences in the modelled transport, especially inter-hemispheric exchange rates and tropical convective mixing. Estimates of the seasonal cycle in N2O emissions are also sensitive to errors in modelled stratosphere-to-troposphere transport in the tropics and southern extratropics. Overall, the results show a convergence in the global and regional emissions compared to previous independent studies.


2007 ◽  
Vol 7 (11) ◽  
pp. 2775-2787 ◽  
Author(s):  
N. Glatthor ◽  
T. von Clarmann ◽  
H. Fischer ◽  
B. Funke ◽  
U. Grabowski ◽  
...  

Abstract. We use limb emission spectra of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard the ENVIronmental SATellite (ENVISAT) to derive the first global distribution of peroxyacetyl nitrate (PAN) in the upper troposphere. PAN is generated in tropospheric air masses polluted by fuel combustion or biomass burning and acts as a reservoir and carrier of NOx in the cold free troposphere. PAN exhibits continuum-like broadband structures in the mid-infrared region and was retrieved in a contiguous analysis window covering the wavenumber region 775–800 cm−1. The interfering species CCl4, HCFC-22, H2O, ClONO2, CH3CCl3 and C2H2 were fitted along with PAN, whereas pre-fitted profiles were used to model the contribution of other contaminants like ozone. Sensitivity tests consisting in retrieval without consideration of PAN demonstrated the existence of PAN signatures in MIPAS spectra obtained in polluted air masses. The analysed dataset consists of 10 days between 4 October and 1 December 2003. This period covers the end of the biomass burning season in South America and South and East Africa, in which generally large amounts of pollutants are produced and distributed over wide areas of the southern hemispheric free troposphere. Indeed, elevated PAN amounts of 200–700 pptv were measured in a large plume extending from Brasil over the Southern Atlantic, Central and South Africa, the South Indian Ocean as far as Australia at altitudes between 8 and 16 km. Enhanced PAN values were also found in a much more restricted area between northern subtropical Africa and India. The most significant northern midlatitude PAN signal was detected in an area at 8 km altitude extending from China into the Chinese Sea. The average mid and high latitude PAN amounts found at 8 km were around 125 pptv in the northern, but only between 50 and 75 pptv in the southern hemisphere. The PAN distribution found in the southern hemispheric tropics and subtropics is highly correlated with the jointly fitted acetylene (C2H2), which is another pollutant produced by biomass burning, and agrees reasonably well with the CO plume detected during end of September 2003 at the 275 hPa level (~10 km) by the Measurement of Pollution in the Troposphere (MOPITT) instrument on the Terra satellite. Similar southern hemispheric PAN amounts were also observed by previous airborne measurements performed in September/October 1992 and 1996 above the South Atlantic and the South Pacific, respectively.


2007 ◽  
Vol 7 (1) ◽  
pp. 1391-1420 ◽  
Author(s):  
N. Glatthor ◽  
T. von Clarmann ◽  
H. Fischer ◽  
B. Funke ◽  
U. Grabowski ◽  
...  

Abstract. We use limb emission spectra of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard the ENVIronmental SATellite (ENVISAT) to derive the first global distribution of peroxyacetyl nitrate (PAN) in the upper troposphere. PAN is generated in tropospheric air masses polluted by fuel combustion or biomass burning and acts as a reservoir and carrier of NOx in the cold free troposphere. Since PAN exhibits continuum-like broadband structures in the mid-infrared region, we have applied a contiguous analysis window covering the wavenumber region 775–800 cm−1 for retrieval. The interfering species CCl4, HCFC-22, H2O, ClONO2, CH3CCl3 and C2H2 were fitted along with PAN, whereas pre-fitted profiles were used to model the contribution of other contaminants like ozone. Sensitivity tests consisting in retrieval without consideration of PAN have demonstrated the existence of PAN signatures in MIPAS spectra obtained from polluted air masses. The analysed dataset consists of 10 days between 4 October and 1 December 2003. This period covers the end of the biomass burning season in South America and South and East Africa, in which generally large amounts of pollutants are produced and distributed over wide areas in the southern hemispheric free troposphere. Elevated PAN amounts of 200–700 pptv were measured in a large plume extending from Brasil over the Southern Atlantic, Central and South Africa, the South Indian Ocean as far as Australia at altitudes between 8 and 16 km. Enhanced PAN values were also found in a much more restricted area between northern subtropical Africa and India. The most significant northern midlatitude PAN signal in MIPAS data is an area extending at 8 km altitude from China into the Chinese Sea. The average mid and high latitude PAN amounts found at 8 km were around 125 pptv in the northern, but only between 75 and 50 pptv in the southern hemisphere. The PAN distribution found in the southern hemispheric tropics and subtropics is highly correlated with the jointly fitted acetylene (C2H2), which is another pollutant produced by biomass burning, and agrees reasonably well with the CO plume detected during end of September 2003 at the 275 hPa level (~10 km) by the Measurement of Pollution in the Troposphere (MOPITT) instrument on the Terra satellite. Similar southern hemispheric PAN amounts were also observed by previous airborne measurements performed in September/October 1992 and 1996 above the South Atlantic and the South Pacific, respectively.


2021 ◽  
Author(s):  
Michael Höpfner ◽  
Oliver Kirner ◽  
Gerald Wetzel ◽  
Björn-Martin Sinnhuber ◽  
Florian Haenel ◽  
...  

Abstract. We present the first observational dataset of vertically resolved global stratospheric BrONO2 distributions from July 2002 until April 2012, and compare them to results of the atmospheric chemical climate model EMAC. The retrieved distributions are based on space-borne measurements of infrared limb-emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. The derived vertical profiles of BrONO2 volume mixing ratios represent 10° latitude bins and three-day means, separated into sunlit and observations in the dark. The estimated uncertainties are around 1–4 pptv caused by spectral noise for single profiles as well as for further parameter and systematic errors which may not improve by averaging. Vertical resolutions range from 3 to 8 km between 15 and 35 km altitude. All leading modes of spatial and temporal variability of stratospheric BrONO2 in the observations are well replicated by the model simulations: the large diurnal variability, the low values during polar winter as well as the maximum values at mid- and high latitudes during summer. Three major differences between observations and model results are observed: (1) a model underestimation of enhanced BrONO2 in the polar winter stratosphere above about 30 km of up to 15 pptv, (2) up to 8 pptv higher modelled values than observed globally in the lower stratosphere up to 25 km most obvious during night, and (3) up to 5 pptv lower modelled concentrations at tropical latitudes between 27 and 32 km during sunlit conditions. (1) is explained by the model missing enhanced NOx produced in the mesosphere and lower thermosphere subsiding at high latitudes in winter. This is the first time that observational evidence for enhancement of BrONO2 caused by mesospheric NOx production is reported. The other major inconsistencies (2,3) between EMAC model results and observations are studied by sensitivity runs with a 1d model. These tentatively hint to a model underestimation of heterogeneous loss of BrONO2 in the lower stratosphere, a too low simulated production of BrONO2 during day as well as strongly underestimated BrONO2 volume mixing ratios when loss via reaction with O(3P) is considered additionally to photolysis. However, considering the uncertainty ranges of model parameters and of measurements, an unambiguous identification of the causes for the differences remains difficult. The observations have also been used to derive the total stratospheric bromine content relative to years of stratospheric entry between 1997 and 2007. With an average value of 21.2 ± 1.4 pptv of Bry at mid-latitudes where the modelled adjustment from BrONO2 to Bry is lowest, the MIPAS data agree with estimates of Bry derived from observations of BrO as well as from MIPAS-Balloon measurements of BrONO2.


2018 ◽  
Vol 11 (4) ◽  
pp. 2135-2149 ◽  
Author(s):  
Carlo Arosio ◽  
Alexei Rozanov ◽  
Elizaveta Malinina ◽  
Kai-Uwe Eichmann ◽  
Thomas von Clarmann ◽  
...  

Abstract. This study describes a retrieval algorithm developed at the University of Bremen to obtain vertical profiles of ozone from limb observations performed by the Ozone Mapper and Profiler Suite (OMPS). This algorithm is based on the technique originally developed for use with data from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument. As both instruments make limb measurements of the scattered solar radiation in the ultraviolet (UV) and visible (Vis) spectral ranges, an underlying objective of the study is to obtain consolidated and consistent ozone profiles from the two satellites and to produce a combined data set. The retrieval algorithm uses radiances in the UV and Vis wavelength ranges normalized to the radiance at an upper tangent height to obtain ozone concentrations in the altitude range of 12–60 km. Measurements at altitudes contaminated by clouds in the instrument field of view are identified and filtered out. An independent aerosol retrieval is performed beforehand and its results are used to account for the stratospheric aerosol load in the ozone inversion. The typical vertical resolution of the retrieved profiles varies from  ∼  2.5 km at lower altitudes ( < 30 km) to  ∼  1.5 km (about 45 km) and becomes coarser at upper altitudes. The retrieval errors resulting from the measurement noise are estimated to be 1–4 % above 25 km, increasing to 10–30 % in the upper troposphere. OMPS data are processed for the whole of 2016. The results are compared with the NASA product and validated against profiles derived from passive satellite observations or measured in situ by balloon-borne sondes. Between 20 and 60 km, OMPS ozone profiles typically agree with data from the Microwave Limb Sounder (MLS) v4.2 within 5–10 %, whereas in the lower altitude range the bias becomes larger, especially in the tropics. The comparison of OMPS profiles with ozonesonde measurements shows differences within ±5 % between 13 and 30 km at northern middle and high latitudes. At southern middle and high latitudes, an agreement within 5–7 % is also achieved in the same altitude range. An unexpected bias of approximately 10–20 % is detected in the lower tropical stratosphere. The processing of the 2013 data set using the same retrieval settings and its validation against ozonesondes reveals a much smaller bias; a possible reason for this behaviour is discussed.


Author(s):  
Johan Lundberg

AbstractTheories of inter-jurisdictional tax and yardstick competition assume that the tax decisions of one jurisdiction will influence the tax decisions of other jurisdictions. This paper empirically addresses the issue of horizontal dependence in local personal income tax rates across jurisdictions. Based on a large data set covering Swedish municipalities over a period of 14 years, we test for interactions across municipalities that share a common border, across municipalities within a distance of 100 km of each other, and across municipalities with similar political representation in the local council. We also test the hypothesis that the tax rate of relatively larger municipalities has a greater influence on their neighbors' tax rate compared to the influence of their smaller neighbors. Our results suggest that when lagged tax rates are controlled for, the horizontal correlation across municipalities that share a common border or are within a distance of 100 km from each other becomes insignificant. This result is of importance as it suggests that lagged tax rates should be included or at least tested for when testing for horizontal interactions or mimicking in local tax rates. However, our results support the hypothesis of horizontal interactions across municipalities that share a common border when the influence of neighboring municipalities is also weighted by their relative population size, i.e. relatively larger neighbors tend to have a greater impact on their neighbor's tax rates than their relatively smaller neighbors. This is of importance as it suggests that distance or proximity matters, although only in combination with the relative population size. We also find some evidence of horizontal dependence across municipalities with similar political preferences.


2015 ◽  
Vol 8 (2) ◽  
pp. 941-963 ◽  
Author(s):  
T. Vlemmix ◽  
F. Hendrick ◽  
G. Pinardi ◽  
I. De Smedt ◽  
C. Fayt ◽  
...  

Abstract. A 4-year data set of MAX-DOAS observations in the Beijing area (2008–2012) is analysed with a focus on NO2, HCHO and aerosols. Two very different retrieval methods are applied. Method A describes the tropospheric profile with 13 layers and makes use of the optimal estimation method. Method B uses 2–4 parameters to describe the tropospheric profile and an inversion based on a least-squares fit. For each constituent (NO2, HCHO and aerosols) the retrieval outcomes are compared in terms of tropospheric column densities, surface concentrations and "characteristic profile heights" (i.e. the height below which 75% of the vertically integrated tropospheric column density resides). We find best agreement between the two methods for tropospheric NO2 column densities, with a standard deviation of relative differences below 10%, a correlation of 0.99 and a linear regression with a slope of 1.03. For tropospheric HCHO column densities we find a similar slope, but also a systematic bias of almost 10% which is likely related to differences in profile height. Aerosol optical depths (AODs) retrieved with method B are 20% high compared to method A. They are more in agreement with AERONET measurements, which are on average only 5% lower, however with considerable relative differences (standard deviation ~ 25%). With respect to near-surface volume mixing ratios and aerosol extinction we find considerably larger relative differences: 10 ± 30, −23 ± 28 and −8 ± 33% for aerosols, HCHO and NO2 respectively. The frequency distributions of these near-surface concentrations show however a quite good agreement, and this indicates that near-surface concentrations derived from MAX-DOAS are certainly useful in a climatological sense. A major difference between the two methods is the dynamic range of retrieved characteristic profile heights which is larger for method B than for method A. This effect is most pronounced for HCHO, where retrieved profile shapes with method A are very close to the a priori, and moderate for NO2 and aerosol extinction which on average show quite good agreement for characteristic profile heights below 1.5 km. One of the main advantages of method A is the stability, even under suboptimal conditions (e.g. in the presence of clouds). Method B is generally more unstable and this explains probably a substantial part of the quite large relative differences between the two methods. However, despite a relatively low precision for individual profile retrievals it appears as if seasonally averaged profile heights retrieved with method B are less biased towards a priori assumptions than those retrieved with method A. This gives confidence in the result obtained with method B, namely that aerosol extinction profiles tend on average to be higher than NO2 profiles in spring and summer, whereas they seem on average to be of the same height in winter, a result which is especially relevant in relation to the validation of satellite retrievals.


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