scholarly journals Carbonaceous material in aerosol particles in the lower stratosphere and tropopause region

2007 ◽  
Vol 112 (D4) ◽  
Author(s):  
D. M. Murphy ◽  
D. J. Cziczo ◽  
P. K. Hudson ◽  
D. S. Thomson
Keyword(s):  
Lower Stratosphere ◽  
Aerosol Particles ◽  
Carbonaceous Material ◽  
Tropopause Region

Distinct particle modes in the lower stratosphere constrain secondary aerosol chemistry and gas-phase concentrations

2021 ◽  
Author(s):  
Daniel Murphy ◽  
Karl Froyd ◽  
Greg Schill ◽  
Charles Brock ◽  
Agnieszka Kupc ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Gas Phase ◽  
Lower Stratosphere ◽  
Aerosol Particles ◽  
Organic Content ◽  
Aerosol Chemistry ◽  
Volatile Organics ◽  
Organic Sulfate ◽  
Concentration Limits ◽  
Distinct Particle

<p>There are distinct types of aerosol particles in the lower stratosphere. Stratospheric sulfuric acid particles with and without meteoric metals coexist with mixed organic-sulfate particles that originated in the troposphere. That these particles remain distinct has important implications for aerosol chemistry and the concentrations of several gas-phase species. Neither semi-volatile organics nor ammonia can be in equilibrium with the gas phase. The gas-phase concentrations of semi-volatile organics and ammonia must be very low, or else the sulfuric acid particles would not stay so pure. The upper concentration limits are around a pptv. Yet the sulfuric acid particles in the Northern Hemisphere show a very small but measurable uptake of organics and ammonia, indicating non-zero gas-phase concentrations of those species. Finally, the organic-sulfate particles must be resistant to photochemical loss, or else they would no longer retain their organic content.</p>

scholarly journals Tropical convection regimes in climate models: evaluation with satellite observations

2017 ◽  
Author(s):  
Andrea K. Steiner ◽  
Bettina C. Lackner ◽  
Mark A. Ringer
Keyword(s):  
Climate Models ◽  
Lower Stratosphere ◽  
Deep Convection ◽  
Atmospheric Temperature ◽  
Tropical Convection ◽  
Specific Humidity ◽  
Moist Convection ◽  
Tropopause Region ◽  
Tropical Troposphere ◽  
Unique Source

Abstract. High quality observations are powerful tools for the evaluation of climate models towards improvement and reduction of uncertainty. Particularly at low latitudes, the most uncertain aspect lies in the representation of moist convection and interaction with dynamics, where rising motion is tied to deep convection and sinking motion to dry regimes. Since humidity is closely coupled with temperature feedbacks in the tropical troposphere a proper representation of this region is essential. Here we demonstrate the evaluation of atmospheric climate models with satellite-based observations from Global Positioning System (GPS) radio occultation (RO), which feature high vertical resolution and accuracy in the troposphere to lower stratosphere. We focus on the representation of the vertical atmospheric structure in tropical convection regimes, defined by high updraft velocity over warm surfaces, and investigate atmospheric temperature and humidity profiles. Results reveal that some models do not fully capture convection regions, particularly over land, and only partly represent high updraft or downdraft velocities. Models show large biases in tropical mean temperature of more than 4 K in the tropopause region and the lower stratosphere. Reasonable agreement with observations is given in mean specific humidity in the lower to mid-troposphere. In moist convection regions, models tend to underestimate moisture by 10 % to 30 % over oceans whereas in dry downdraft regions they overestimate moisture by 100 %. Our findings provide evidence that RO observations are a unique source of information, with a range of further atmospheric variables to be exploited, for the evaluation and advancement of next generation climate models.

scholarly journals A reassessment of the discrepancies in the annual variation of <i>δ</i>D-H<sub>2</sub>O in the tropical lower stratosphere between the MIPAS and ACE-FTS satellite data sets

2020 ◽  
Vol 13 (1) ◽  
pp. 287-308
Author(s):  
Stefan Lossow ◽  
Charlotta Högberg ◽  
Farahnaz Khosrawi ◽  
Gabriele P. Stiller ◽  
Ralf Bauer ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Annual Variation ◽  
Lower Stratosphere ◽  
Michelson Interferometer ◽  
Tape Recorder ◽  
Data Sets ◽  
Altitude Effect ◽  
Data Set ◽  
Tropical Tropopause ◽  
Tropopause Region

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.

Water vapour in the Upper Troposphere and Lower Stratosphere (UTLS): A new vertically resolved dataset from limb and nadir satellite observations

2020 ◽  
Author(s):  
Hao Ye ◽  
Michaela Hegglin ◽  
Martina Krämer ◽  
Christian Rolf ◽  
Alexandra Laeng ◽  
...  
Keyword(s):  
Climate Change ◽  
Water Vapour ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Chemical Properties ◽  
Upper Troposphere ◽  
Data Record ◽  
Tropopause Region ◽  
Quality Water

&lt;p&gt;Water vapour in the upper troposphere and lower stratosphere (UTLS) has a significant impact both on the radiative and chemical properties of the atmosphere. Reliable water vapour observations are essential for the evaluation of the accuracy of UTLS water vapour from model simulations, and thereafter of the contribution to the global radiative forcing and climate change. Limb-viewing and nadir satellites provide high quality water vapour observations above the lower stratosphere and below the upper troposphere, respectively, but show large uncertainties in the tropopause region.&lt;span&gt;&amp;#160; &lt;/span&gt;Within the ESA Water Vapour Climate Change Initiative, we have developed a new scheme to optimally estimate water vapour profiles in the UTLS and in particular across the tropopause, by merging observations from a set of limb and nadir satellites from 2010 to 2014. The new data record of vertically resolved water vapour is validated against the aircraft in-situ water vapour observations from the JULIA database and frostpoint hydrometer records from WAVAS. Furthermore, the new data record is used to evaluate the UTLS water vapour distribution and interannual variations from chemistry-climate model (CCM) simulations and the ERA-5 reanalysis.&lt;/p&gt;

scholarly journals Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N

2021 ◽  
Vol 21 (2) ◽  
pp. 989-1013
Author(s):  
Johannes Schneider ◽  
Ralf Weigel ◽  
Thomas Klimach ◽  
Antonis Dragoneas ◽  
Oliver Appel ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Lower Stratosphere ◽  
Aerosol Particles ◽  
Potential Temperature ◽  
Polar Vortex ◽  
Stratospheric Aerosol ◽  
Loss Mechanism ◽  
Lower Altitude ◽  
Tropospheric Aerosol ◽  
Meteoric Material

Abstract. We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (> 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (< 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.

scholarly journals When does new particle formation not occur in the upper troposphere?

2007 ◽  
Vol 7 (5) ◽  
pp. 14209-14232 ◽  
Author(s):  
D. R. Benson ◽  
L.-H. Young ◽  
S.-H. Lee ◽  
T. L. Campos ◽  
D. C. Rogers ◽  
...  
Keyword(s):  
Case Studies ◽  
Surface Area ◽  
Lower Stratosphere ◽  
Vertical Motion ◽  
Particle Formation ◽  
New Particle Formation ◽  
Upper Troposphere ◽  
Surface Areas ◽  
Total Particle ◽  
Tropopause Region

Abstract. Recent aircraft studies showed that new particle formation is very active in the free troposphere and lower stratosphere. And, these observations lead to a new question: when does new particle formation not occur? Here, we provide case studies to show how convection and surface area affect new particle formation in the upper troposphere, using the measured aerosol size distributions during the NSF/NCAR GV Progressive Science Missions in December 2005. There were ten research flights, including three days of nighttime experiments, at latitudes from 18 to 52° N and altitudes up to 14 km. About 78% of the total samples showed the new particle formation feature with number concentrations of particles with diameters from 4 to 9 nm, 670±1270 cm−3, and the total particle number concentrations with diameters from 4 to 2000 nm, 920±1470 cm−3. Our case studies show that new particle formation was closely associated with convection and low surface areas of preexisting aerosol particles (<4 μm² cm−3). On the other hand, for the cases where no new particle formation events were observed, air masses usually did not experience a vertical motion and air often originated from either the upper troposphere or lower stratosphere where precursor concentrations are relatively low; in addition, it was also a general trend that non-event cases also had higher surface areas (~16 μm² cm−3). These observations are consistent with other observations during the Progressive Science Missions (Young et al., 2007). Because of the lower temperatures in this region (T<250 K), nucleation is thermodynamically favorable; but because of low aerosol precursor concentrations, nucleation is sensitive to aerosol precursor concentration and surface area. Under such conditions, convection (which brings higher concentrations of aerosol precursors and water vapor to higher altitudes) and low surface area play critical roles on whether new particle formation takes place or not. Latitude dependence of new particles also shows higher particle concentrations in the midlatitude tropopause region than in the subtropics, consistent with Hermann et al. (2003).

scholarly journals Impact of aircraft NO<sub>x</sub> emissions on the atmosphere – tradeoffs to reduce the impact

2005 ◽  
Vol 5 (6) ◽  
pp. 12255-12311 ◽  
Author(s):  
M. Gauss ◽  
I. S. A. Isaksen ◽  
D. S. Lee ◽  
O. A. Søvde
Keyword(s):  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Reactive Nitrogen ◽  
Chemical Transport Model ◽  
Reference Case ◽  
Northern Latitudes ◽  
Tropopause Region ◽  
Eu Project ◽  
The Impact

Abstract. Within the EU-project TRADEOFF, the impact of NOx (=NO+NO2) emissions from subsonic aviation upon the chemical composition of the atmosphere has been calculated with focus on changes in reactive nitrogen, ozone, and the chemical lifetime of methane. We apply a 3-D chemical transport model that includes comprehensive chemistry for both the troposphere and the stratosphere and uses various aircraft emission scenarios developed during TRADEOFF for the year 2000. The environmental effects of enhanced air traffic along polar routes and of possible changes in cruising altitude are investigated. In the reference case the model predicts aircraft-induced maximum increases of zonal-mean NOy (=total reactive nitrogen) between 156 pptv (August) and 322 pptv (May) in the tropopause region of the Northern Hemisphere. Resulting maximum increases in zonal-mean ozone vary between 3.1 ppbv in September and 7.7 ppbv in June. The lifetime of methane is calculated to decrease by 0.71%, inducing a radiative forcing of −6.4 mW/m2. Enhanced use of polar routes implies significantly larger zonal-mean ozone increases in high Northern latitudes during summer, while the effect is negligible in winter. Lowering the flight altitude leads to smaller ozone increase in the lower stratosphere and upper troposphere, and to larger ozone increase at lower altitudes. Regarding total ozone change, the degree of cancellation between these two effects depends on latitude and season, but annually and globally averaged the stratospheric decrease dominates, mainly due to washout of NOy in the troposphere, which weakens the tropospheric increase. Raising flight altitudes increases the ozone burden both in the troposphere and the lower stratosphere, primarily due to a more efficient accumulation of pollutants in the stratosphere.

scholarly journals Tropical convection regimes in climate models: evaluation with satellite observations

2018 ◽  
Vol 18 (7) ◽  
pp. 4657-4672 ◽  
Author(s):  
Andrea K. Steiner ◽  
Bettina C. Lackner ◽  
Mark A. Ringer
Keyword(s):  
Climate Models ◽  
Lower Stratosphere ◽  
Deep Convection ◽  
Atmospheric Temperature ◽  
Tropical Convection ◽  
Specific Humidity ◽  
Moist Convection ◽  
Tropopause Region ◽  
Tropical Troposphere ◽  
Unique Source

Abstract. High-quality observations are powerful tools for the evaluation of climate models towards improvement and reduction of uncertainty. Particularly at low latitudes, the most uncertain aspect lies in the representation of moist convection and interaction with dynamics, where rising motion is tied to deep convection and sinking motion to dry regimes. Since humidity is closely coupled with temperature feedbacks in the tropical troposphere, a proper representation of this region is essential. Here we demonstrate the evaluation of atmospheric climate models with satellite-based observations from Global Positioning System (GPS) radio occultation (RO), which feature high vertical resolution and accuracy in the troposphere to lower stratosphere. We focus on the representation of the vertical atmospheric structure in tropical convection regimes, defined by high updraft velocity over warm surfaces, and investigate atmospheric temperature and humidity profiles. Results reveal that some models do not fully capture convection regions, particularly over land, and only partly represent strong vertical wind classes. Models show large biases in tropical mean temperature of more than 4 K in the tropopause region and the lower stratosphere. Reasonable agreement with observations is given in mean specific humidity in the lower to mid-troposphere. In moist convection regions, models tend to underestimate moisture by 10 to 40 % over oceans, whereas in dry downdraft regions they overestimate moisture by 100 %. Our findings provide evidence that RO observations are a unique source of information, with a range of further atmospheric variables to be exploited, for the evaluation and advancement of next-generation climate models.

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