scholarly journals Measurements of NO, NO<sub>y</sub>, N<sub>2</sub>O, and O<sub>3</sub> during SPURT: implications for transport and chemistry in the lowermost stratosphere

2005 ◽  
Vol 5 (5) ◽  
pp. 8649-8688 ◽  
Author(s):  
M. I. Hegglin ◽  
D. Brunner ◽  
Th. Peter ◽  
P. Hoor ◽  
H. Fischer ◽  
...  

Abstract. We present measurements of NO, NOy, O3, and N2O within the lowermost stratosphere (LMS) over Europe obtained during the SPURT project. The measurements cover each of the four seasons during two years between November 2001 and July 2003, and probe the entire altitude and latitude range of the LMS: from 5° N to 85° N equivalent latitude, and from 290 to 375 K potential temperature. The measurements represent a comprehensive data set of these tracers and reveal atmospheric transport processes that influence tracer distributions in the LMS. Mean mixing ratios of stratospheric tracers in equivalent latitude-potential temperature coordinates show a clear seasonal cycle related to the Brewer-Dobson circulation with highest values in spring and lowest values in autumn. Vertical profiles show strong gradients at the extratropical tropopause suggesting that vertical (cross-isentropic) mixing is reduced above the tropopause. Mixing along isentropes is also strongly reduced since pronounced meridional gradients are found on potential temperature surfaces in the LMS. Concurrent large gradients in PV in the vertical and in the meridional direction horizontally suggest the presence of a transport and mixing barrier. Well above the tropopause distinguished seasonal cycles were found in the correlation slopes ΔO3/ΔN2O and ΔNOy/ΔN2O. Smallest slopes found during spring indicate chemically aged stratospheric air originating from high altitudes and latitudes. The slopes are larger in summer and autumn suggesting that a substantial fraction of air takes a 'short-cut' from the tropical tropopause region into the extratropical LMS. The comparison of measured NO with critical NO values at which net ozone production changes from negative to positive implies a net ozone production up to 20 K above the local tropopause in winter, increasing during spring and summer to up to 50 K in autumn. Above this height NO values favor ozone destruction.

2006 ◽  
Vol 6 (5) ◽  
pp. 1331-1350 ◽  
Author(s):  
M. I. Hegglin ◽  
D. Brunner ◽  
T. Peter ◽  
P. Hoor ◽  
H. Fischer ◽  
...  

Abstract. We present measurements of NO, NOy, O3, and N2O within the lowermost stratosphere (LMS) over Europe obtained during the SPURT project. The measurements cover all seasons between November 2001 and July 2003. They span a broad band of latitudes from 30° N to 75° N and a potential temperature range from 290 to 380 K. The measurements represent a comprehensive data set of these tracers and reveal atmospheric transport processes that influence tracer distributions in the LMS. Median mixing ratios of stratospheric tracers in equivalent latitude-potential temperature coordinates show a clear seasonal cycle related to the Brewer-Dobson circulation, with highest values in spring and lowest values in autumn. Vertical tracer profiles show strong gradients at the extratropical tropopause, suggesting that vertical (cross-isentropic) mixing is reduced above the tropopause. Pronounced meridional gradients in the tracer mixing ratios are found on potential temperature surfaces in the LMS. This suggests strongly reduced mixing along isentropes. Concurrent large gradients in static stability in the vertical direction, and of PV in the meridional direction, suggest the presence of a mixing barrier. Seasonal cycles were found in the correlation slopes ΔO3/ΔN2O and ΔNOy/ΔN2O well above the tropopause. Absolute slope values are smallest in spring indicating chemically aged stratospheric air originating from high altitudes and latitudes. Larger values were measured in summer and autumn suggesting that a substantial fraction of air takes a "short-cut" from the tropical tropopause region into the extratropical LMS. The seasonal change in the composition of the LMS has direct implications for the ozone chemistry in this region. Comparisons of measured NO with the critical NO value at which net ozone production changes from negative to positive, imply ozone production up to 20 K above the local tropopause in spring, up to 30 K in summer, and up to 40 K in autumn. Above these heights, and in winter, net ozone production is negative.


2006 ◽  
Vol 6 (2) ◽  
pp. 283-301 ◽  
Author(s):  
A. Engel ◽  
H. Bönisch ◽  
D. Brunner ◽  
H. Fischer ◽  
H. Franke ◽  
...  

Abstract. During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature-equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.


2005 ◽  
Vol 5 (4) ◽  
pp. 5081-5126
Author(s):  
A. Engel ◽  
H. Bönisch ◽  
D. Brunner ◽  
H. Fischer ◽  
H. Franke ◽  
...  

Abstract. During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature – equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.


2004 ◽  
Vol 4 (5) ◽  
pp. 1427-1442 ◽  
Author(s):  
P. Hoor ◽  
C. Gurk ◽  
D. Brunner ◽  
M. I. Hegglin ◽  
H. Wernli ◽  
...  

Abstract. We present airborne in-situ trace gas measurements which were performed on eight campaigns between November 2001 and July 2003 during the SPURT-project (SPURenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region). The measurements on a quasi regular basis allowed an overview of the seasonal variations of the trace gas distribution in the tropopause region over Europe from 35°-75°N to investigate the influence of transport and mixing across the extratropical tropopause on the lowermost stratosphere. From the correlation of CO and O3 irreversible mixing of tropospheric air into the lowermost stratosphere is identified. The CO distribution indicates that transport and subsequent mixing of tropospheric air across the extratropical tropopause predominantly affects a layer, which closely follows the shape of the local tropopause. In addition, the seasonal cycle of CO2 illustrates the strong coupling of that layer to the extratropical troposphere. Both, horizontal gradients of CO on isentropes as well as the CO-O3-distribution in the lowermost stratosphere reveal that the influence of quasi-horizontal transport and subsequent mixing weakens with distance from the local tropopause. The mixing layer extends to about 25 K in potential temperature above the local tropopause exhibiting only a weak seasonality. However, at large distances from the tropopause a significant influence of tropospheric air is still evident. The relation between N2O and CO2 indicates that a significant contribution of air originating from the tropical tropopause contributes to the background air in the extratropical lowermost stratosphere.


2011 ◽  
Vol 11 (1) ◽  
pp. 407-419 ◽  
Author(s):  
F. Ploeger ◽  
S. Fueglistaler ◽  
J.-U. Grooß ◽  
G. Günther ◽  
P. Konopka ◽  
...  

Abstract. We explore the potential of ozone observations to constrain transport processes in the tropical tropopause layer (TTL), and contrast it with insights that can be obtained from water vapour. Global fields from Halogen Occultation Experiment (HALOE) and in-situ observations are predicted using a backtrajectory approach that captures advection, instantaneous freeze-drying and photolytical ozone production. Two different representations of transport (kinematic and diabatic 3-month backtrajectories based on ERA-Interim data) are used to evaluate the sensitivity to differences in transport. Results show that mean profiles and seasonality of both tracers can be reasonably reconstructed. Water vapour predictions are similar for both transport representations, but predictions for ozone are systematically higher for kinematic transport. Compared to global HALOE observations, the diabatic model prediction underestimates the vertical ozone gradient. Comparison of the kinematic prediction with observations obtained during the tropical SCOUT-O3 campaign shows a large high bias above 390 K potential temperature. We show that ozone predictions and vertical dispersion of the trajectories are highly correlated, rendering ozone an interesting tracer for aspects of transport to which water vapour is not sensitive. We show that dispersion and mean upwelling have similar effects on ozone profiles, with slower upwelling and larger dispersion both leading to higher ozone concentrations. Analyses of tropical upwelling based on mean transport characteristics, and model validation have to take into account this ambiguity between tropical ozone production and in-mixing from the stratosphere. In turn, ozone provides constraints on transport in the TTL and lower stratosphere that cannot be obtained from water vapour.


2013 ◽  
Vol 13 (22) ◽  
pp. 11221-11234 ◽  
Author(s):  
F. Arfeuille ◽  
B. P. Luo ◽  
P. Heckendorn ◽  
D. Weisenstein ◽  
J. X. Sheng ◽  
...  

Abstract. In terms of atmospheric impact, the volcanic eruption of Mt. Pinatubo (1991) is the best characterized large eruption on record. We investigate here the model-derived stratospheric warming following the Pinatubo eruption as derived from SAGE II extinction data including recent improvements in the processing algorithm. This method, termed SAGE_4λ, makes use of the four wavelengths (385, 452, 525 and 1024 nm) of the SAGE II data when available, and uses a data-filling procedure in the opacity-induced "gap" regions. Using SAGE_4λ, we derived aerosol size distributions that properly reproduce extinction coefficients also at much longer wavelengths. This provides a good basis for calculating the absorption of terrestrial infrared radiation and the resulting stratospheric heating. However, we also show that the use of this data set in a global chemistry–climate model (CCM) still leads to stronger aerosol-induced stratospheric heating than observed, with temperatures partly even higher than the already too high values found by many models in recent general circulation model (GCM) and CCM intercomparisons. This suggests that the overestimation of the stratospheric warming after the Pinatubo eruption may not be ascribed to an insufficient observational database but instead to using outdated data sets, to deficiencies in the implementation of the forcing data, or to radiative or dynamical model artifacts. Conversely, the SAGE_4λ approach reduces the infrared absorption in the tropical tropopause region, resulting in a significantly better agreement with the post-volcanic temperature record at these altitudes.


2010 ◽  
Vol 10 (8) ◽  
pp. 3615-3627 ◽  
Author(s):  
C. D. Homan ◽  
C. M. Volk ◽  
A. C. Kuhn ◽  
A. Werner ◽  
J. Baehr ◽  
...  

Abstract. We present airborne in situ measurements made during the AMMA (African Monsoon Multidisciplinary Analysis)/SCOUT-O3 campaign between 31 July and 17 August 2006 on board the M55 Geophysica aircraft, based in Ouagadougou, Burkina Faso. CO2 and N2O were measured with the High Altitude Gas Analyzer (HAGAR), CO was measured with the Cryogenically Operated Laser Diode (COLD) instrument, and O3 with the Fast Ozone ANalyzer (FOZAN). We analyse the data obtained during five local flights to study the dominant transport processes controlling the tropical tropopause layer (TTL, here ~350–375 K) and lower stratosphere above West-Africa: deep convection up to the level of main convective outflow, overshooting of deep convection, and horizontal inmixing across the subtropical tropopause. Besides, we examine the morphology of the stratospheric subtropical barrier. Except for the flight of 13 August, distinct minima in CO2 mixing ratios indicate convective outflow of boundary layer air in the TTL. The CO2 profiles show that the level of main convective outflow was mostly located at potential temperatures between 350 and 360 K, and for 11 August reached up to 370 K. While the CO2 minima indicate quite significant convective influence, the O3 profiles suggest that the observed convective signatures were mostly not fresh, but of older origin (several days or more). When compared with the mean O3 profile measured during a previous campaign over Darwin in November 2005, the O3 minimum at the main convective outflow level was less pronounced over Ouagadougou. Furthermore O3 mixing ratios were much higher throughout the whole TTL and, unlike over Darwin, rarely showed low values observed in the regional boundary layer. Signatures of irreversible mixing following overshooting of convective air were scarce in the tracer data. Some small signatures indicative of this process were found in CO2 profiles between 390 and 410 K during the flights of 4 and 8 August, and in CO data at 410 K on 7 August. However, the absence of expected corresponding signatures in other tracer data makes this evidence inconclusive, and overall there is little indication from the observations that overshooting convection has a profound impact on gas-phase tracer TTL composition during AMMA. We find the amount of photochemically aged air isentropically mixed into the TTL across the subtropical tropopause to be not significant. Using the N2O observations we estimate the fraction of aged extratropical stratospheric air in the TTL to be 0.0±0.1 up to 370 K during the local flights. Above the TTL this fraction increases to 0.3±0.1 at 390 K. The subtropical barrier, as indicated by the slope of the correlation between N2O and O3 between 415 and 490 K, does not appear as a sharp border between the tropics and extratropics, but rather as a gradual transition region between 10° N and 25° N where isentropic mixing between these two regions may occur.


2020 ◽  
Vol 13 (1) ◽  
pp. 287-308
Author(s):  
Stefan Lossow ◽  
Charlotta Högberg ◽  
Farahnaz Khosrawi ◽  
Gabriele P. Stiller ◽  
Ralf Bauer ◽  
...  

Abstract. The annual variation of δD in the tropical lower stratosphere is a critical indicator for the relative importance of different processes contributing to the transport of water vapour through the cold tropical tropopause region into the stratosphere. Distinct observational discrepancies of the δD annual variation were visible in the works of Steinwagner et al. (2010) and Randel et al. (2012). Steinwagner et al. (2010) analysed MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) observations retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung in Karlsruhe, Germany, in collaboration with the Instituto de Astrofísica de Andalucía in Granada, Spain) processor, while Randel et al. (2012) focused on ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. Here we reassess the discrepancies based on newer MIPAS (IMK/IAA) and ACE-FTS data sets, also showing for completeness results from SMR (Sub-Millimetre Radiometer) observations and a ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg and Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulation (Eichinger et al., 2015b). Similar to the old analyses, the MIPAS data set yields a pronounced annual variation (maximum about 75 ‰), while that derived from the ACE-FTS data set is rather weak (maximum about 25 ‰). While all data sets exhibit the phase progression typical for the tape recorder, the annual maximum in the ACE-FTS data set precedes that in the MIPAS data set by 2 to 3 months. We critically consider several possible reasons for the observed discrepancies, focusing primarily on the MIPAS data set. We show that the δD annual variation in the MIPAS data up to an altitude of 40 hPa is substantially impacted by a “start altitude effect”, i.e. dependency between the lowermost altitude where MIPAS retrievals are possible and retrieved data at higher altitudes. In itself this effect does not explain the differences with the ACE-FTS data. In addition, there is a mismatch in the vertical resolution of the MIPAS HDO and H2O data (being consistently better for HDO), which actually results in an artificial tape-recorder-like signal in δD. Considering these MIPAS characteristics largely removes any discrepancies between the MIPAS and ACE-FTS data sets and shows that the MIPAS data are consistent with a δD tape recorder signal with an amplitude of about 25 ‰ in the lowermost stratosphere.


2004 ◽  
Vol 4 (3) ◽  
pp. 741-756 ◽  
Author(s):  
M. I. Hegglin ◽  
D. Brunner ◽  
H. Wernli ◽  
C. Schwierz ◽  
O. Martius ◽  
...  

Abstract. Within the project SPURT (trace gas measurements in the tropopause region) a variety of trace gases have been measured in situ in order to investigate the role of dynamical and chemical processes in the extra-tropical tropopause region. In this paper we report on a flight on 10 November 2001 leading from Hohn, Germany (52ºN) to Faro, Portugal (37ºN) through a strongly developed deep stratospheric intrusion. This streamer was associated with a large convective system over the western Mediterranean with potentially significant troposphere-to-stratosphere transport. Along major parts of the flight we measured unexpectedly high NOy mixing ratios. Also H2O mixing ratios were significantly higher than stratospheric background levels confirming the extraordinary chemical signature of the probed air masses in the interior of the streamer. Backward trajectories encompassing the streamer enable to analyze the origin and physical characteristics of the air masses and to trace troposphere-to-stratosphere transport. Near the western flank of the intrusion features caused by long range transport, such as tropospheric filaments characterized by sudden drops in the O3 and NOy mixing ratios and enhanced CO and H2O can be reconstructed in great detail using the reverse domain filling technique. These filaments indicate a high potential for subsequent mixing with the stratospheric air. At the south-western edge of the streamer a strong gradient in the NOy and the O3 mixing ratios coincides very well with a sharp gradient in potential vorticity in the ECMWF fields. In contrast, in the interior of the streamer the observed highly elevated NOy and H2O mixing ratios up to a potential temperature level of 365 K and potential vorticity values of maximum 10 PVU cannot be explained in terms of resolved troposphere-to-stratosphere transport along the backward trajectories. Also mesoscale simulations with a High Resolution Model reveal no direct evidence for convective H2O injection up to this level. Elevated H2O mixing ratios in the ECMWF and HRM model are seen only up to about tropopause height at 340 hPa and 270hPa, respectively, well below flight altitude of about 200 hPa. However, forward tracing of the convective influence as identified by satellite brightness temperature measurements and counts of lightning strokes shows that during this part of the flight the aircraft was closely following the border of an air mass which was heavily impacted by convective activity over Spain and Algeria. This is evidence that deep convection at mid-latitudes may have a large impact on the tracer distribution of the lowermost stratosphere reaching well above the thunderstorms anvils as claimed by recent studies using cloud-resolving models.


2020 ◽  
Author(s):  
Meike Rotermund ◽  
Ben Schreiner ◽  
Flora Kluge ◽  
Tilman Hüneke ◽  
Andreas Engel ◽  
...  

&lt;p&gt;Bromine greatly influences the UT/LS ozone concentrations, however the transport of bromine across the tropical tropopause layer and in particular across the extratropical tropopause is not well quantified. Air-borne measurements of atmospheric trace gases such as organic and inorganic bromine along the tropopause are studied during the WISE (Wave-driven ISentropic Exchange) research campaign over the northern Atlantic and western Europe from September 13 - October 21, 2017. The remote sensing instrument mini-DOAS (Differential Optical Absorption Spectroscopy) is mounted on the HALO (High Altitude and LOng range) aircraft and measures BrO (O&lt;sub&gt;3&lt;/sub&gt;, NO&lt;sub&gt;2&lt;/sub&gt; among other trace gases). The novel scaling method is applied to infer the target gas BrO mixing ratios from slant column densities using in-situ O&lt;sub&gt;3&lt;/sub&gt; measurements from the FAIRO instrument (operated by KIT) as the scaling gas. For each flight, the inferred mixing ratios are directly compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulated curtains of the trace gases along the flight path. The partitioning coefficient of inorganic bromine from CLaMS and all relevant organic halogen species and air mass ages (SF&lt;sub&gt;6&lt;/sub&gt;, CO&lt;sub&gt;2&lt;/sub&gt;) from the GhOST-MS instrument (operated by UFra) are used to determine the total bromine budget along the UT/LS. A climatology of organic, inorganic and total bromine is constructed with respect to the extratropical tropopause as well as the air mass ages. This indicates the interplay of bromine transport across the extratropical tropopause and of the transport of air via the lower branch from the tropics as well as potential losses of inorganic bromine by uptake onto and sedimentation of ice particles.&lt;/p&gt;


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