scholarly journals The observation of nitric acid-containing particles in the tropical lower stratosphere

2005 ◽  
Vol 5 (5) ◽  
pp. 10097-10124
Author(s):  
P. J. Popp ◽  
T. P. Marcy ◽  
E. J. Jensen ◽  
B. Kärcher ◽  
D. W. Fahey ◽  
...  

Abstract. Airborne in situ measurements over the eastern Pacific Ocean in January 2004 have revealed a new category of nitric acid (HNO3)-containing particles in the tropical lower stratosphere. These particles are most likely composed of nitric acid trihydrate (NAT). They were intermittently observed in a narrow layer above the tropopause (18±0.1 km) and over a broad geographic extent (>1100 km). In contrast to the background liquid sulfate aerosol, these particles are solid, much larger (1.7–4.7 µm vs. 0.1 µm in diameter), and significantly less abundant (<10-4 cm-3 vs. 10 cm-3). Microphysical trajectory models suggest that the NAT particles grow over a 6–14 day period in supersaturated air that remains close to the tropical tropopause and might be a common feature in the tropics. The small number density of these particles implies a highly selective or slow nucleation process. Understanding the formation of solid NAT particles in the tropics could improve our understanding of stratospheric nucleation processes and, therefore, dehydration and denitrification.

2006 ◽  
Vol 6 (3) ◽  
pp. 601-611 ◽  
Author(s):  
P. J. Popp ◽  
T. P. Marcy ◽  
E. J. Jensen ◽  
B. Kärcher ◽  
D. W. Fahey ◽  
...  

Abstract. Airborne in situ measurements over the eastern Pacific Ocean in January 2004 have revealed a new category of nitric acid (HNO3)-containing particles in the tropical lower stratosphere. These particles are most likely composed of nitric acid trihydrate (NAT). They were intermittently observed in a narrow layer above the tropopause (18±0.1 km) and over a broad geographic extent (>1100 km). In contrast to the background liquid sulfate aerosol, these particles are solid, much larger (1.7-4.7 µm vs. 0.1µm in diameter), and significantly less abundant (<10-4 cm-3 vs. 10 cm-3). Microphysical trajectory models suggest that the NAT particles grow over a 6-14 day period in supersaturated air that remains close to the tropical tropopause and might be a common feature in the tropics. The small number density of these particles implies a highly selective or slow nucleation process. Understanding the formation of solid NAT particles in the tropics could improve our understanding of stratospheric nucleation processes and, therefore, dehydration and denitrification.


2003 ◽  
Vol 3 (4) ◽  
pp. 1083-1091 ◽  
Author(s):  
Th. Peter ◽  
B. P. Luo ◽  
M. Wirth ◽  
C. Kiemle ◽  
H. Flentje ◽  
...  

Abstract. Subvisible cirrus clouds (SVCs) may contribute to dehydration close to the tropical tropopause. The higher and colder SVCs and the larger their ice crystals, the more likely they represent the last efficient point of contact of the gas phase with the ice phase and, hence, the last dehydrating step, before the air enters the stratosphere. The first simultaneous in situ and remote sensing measurements of SVCs were taken during the APE-THESEO campaign in the western Indian ocean in February/March 1999. The observed clouds, termed Ultrathin Tropical Tropopause Clouds (UTTCs), belong to the geometrically and optically thinnest large-scale clouds in the Earth's atmosphere. Individual UTTCs may exist for many hours as an only 200--300 m thick cloud layer just a few hundred meters below the tropical cold point tropopause, covering up to 105 km2. With temperatures as low as 181 K these clouds are prime representatives for defining the water mixing ratio of air entering the lower stratosphere.


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.


2016 ◽  
Vol 16 (18) ◽  
pp. 12273-12286 ◽  
Author(s):  
Sergey M. Khaykin ◽  
Jean-Pierre Pommereau ◽  
Emmanuel D. Riviere ◽  
Gerhard Held ◽  
Felix Ploeger ◽  
...  

Abstract. High-resolution in situ balloon measurements of water vapour, aerosol, methane and temperature in the upper tropical tropopause layer (TTL) and lower stratosphere are used to evaluate the processes affecting the stratospheric water budget: horizontal transport (in-mixing) and hydration by cross-tropopause overshooting updrafts. The obtained in situ evidence of these phenomena are analysed using satellite observations by Aura MLS (Microwave Limb Sounder) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) together with trajectory and transport modelling performed using CLaMS (Chemical Lagrangian Model of the Stratosphere) and HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) model. Balloon soundings were conducted during March 2012 in Bauru, Brazil (22.3° S) in the frame of the TRO-Pico campaign for studying the impact of convective overshooting on the stratospheric water budget. The balloon payloads included two stratospheric hygrometers: FLASH-B (Fluorescence Lyman-Alpha Stratospheric Hygrometer for Balloon) and Pico-SDLA instrument as well as COBALD (Compact Optical Backscatter Aerosol Detector) sondes, complemented by Vaisala RS92 radiosondes. Water vapour vertical profiles obtained independently by the two stratospheric hygrometers are in excellent agreement, ensuring credibility of the vertical structures observed. A signature of in-mixing is inferred from a series of vertical profiles, showing coincident enhancements in water vapour (of up to 0.5 ppmv) and aerosol at the 425 K (18.5 km) level. Trajectory analysis unambiguously links these features to intrusions from the Southern Hemisphere extratropical stratosphere, containing more water and aerosol, as demonstrated by MLS and CALIPSO global observations. The in-mixing is successfully reproduced by CLaMS simulations, showing a relatively moist filament extending to 20° S. A signature of local cross-tropopause transport of water is observed in a particular sounding, performed on a convective day and revealing water vapour enhancements of up to 0.6 ppmv as high as the 404 K (17.8 km) level. These are shown to originate from convective overshoots upwind detected by an S-band weather radar operating locally in Bauru. The accurate in situ observations uncover two independent moisture pathways into the tropical lower stratosphere, which are hardly detectable by space-borne sounders. We argue that the moistening by horizontal transport is limited by the weak meridional gradients of water, whereas the fast convective cross-tropopause transport, largely missed by global models, can have a substantial effect, at least at a regional scale.


2009 ◽  
Vol 9 (6) ◽  
pp. 24587-24628 ◽  
Author(s):  
S. Borrmann ◽  
D. Kunkel ◽  
R. Weigel ◽  
A. Minikin ◽  
T. Deshler ◽  
...  

Abstract. Processes occurring in the tropical upper troposphere and lower stratosphere (UT/LS) are of importance for the global climate, for the stratospheric dynamics and air chemistry, and they influence the global distribution of water vapour, trace gases and aerosols. The mechanisms underlying cloud formation and variability in the UT/LS are of scientific concern as these still are not adequately described and quantified by numerical models. Part of the reasons for this is the scarcity of detailed in-situ measurements in particular from the Tropical Transition Layer (TTL) within the UT/LS. In this contribution we provide measurements of particle number densities and the amounts of non-volatile particles in the submicron size range present in the UT/LS over Southern Brazil, West Africa, and Northern Australia. The data were collected in-situ on board of the Russian high altitude research aircraft M-55 "Geophysica" using the specialised COPAS (COndensation PArticle counting System) instrument during the TROCCINOX (Araçatuba, Brazil, February 2005), the SCOUT-O3 (Darwin, Australia, December 2005), and SCOUT-AMMA (Ouagadougou, Burkina Faso, August 2006) campaigns. The vertical profiles obtained are compared to those from previous measurements from the NASA DC-8 and NASA WB-57F over Costa Rica and other tropical locations between 1999 and 2007. The number density of the submicron particles as function of altitude was found to be remarkably constant (even back to 1987) over the tropical UT/LS altitude band such that a parameterisation suitable for models can be extracted from the measurements. At altitudes corresponding to potential temperatures above 430 K a slight increase of the number densities from 2005/2006 results from the data in comparison to the 1987 to 2007 measurements. The origins of this increase are unknown. By contrast the data from Northern hemispheric mid latitudes do not exhibit such an increase between 1999 and 2006. Vertical profiles of the non-volatile fraction of the submicron particles were also measured by a COPAS channel and are presented here. The resulting profiles of the non-volatile number density fraction show a pronounced maximum of 50% in the tropical TTL over Australia and West Africa. Below and above this fraction is much lower attaining values of 10% and smaller. In the lower stratosphere the fine particles mostly consist of sulphuric acid which is reflected in the low numbers of non-volatile residues measured by COPAS. Without detailed chemical composition measurements the reason for the increase of non-volatile particle fractions cannot yet be given. The long distance transfer flights to Brazil, Australia and West-Africa were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data measured during these transfers represent a "snapshot picture" documenting the status of a significant part of the global UT/LS aerosol (with sizes below 1 μm) at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo) eruption. The corresponding latitudinal distributions of the measured particle number densities are also presented in this paper in order to provide input on the UT/LS background aerosol for modelling purposes.


2011 ◽  
Vol 11 (8) ◽  
pp. 3937-3948 ◽  
Author(s):  
H. Bönisch ◽  
A. Engel ◽  
Th. Birner ◽  
P. Hoor ◽  
D. W. Tarasick ◽  
...  

Abstract. In this paper we present evidence that the observed increase in tropical upwelling after the year 2000 may be attributed to a change in the Brewer-Dobson circulation pattern. For this purpose, we use the concept of transit times derived from residual circulation trajectories and different in-situ measurements of ozone and nitrous dioxide. Observations from the Canadian midlatitude ozone profile record, probability density functions of in-situ N2O observations and a shift of the N2O-O3 correlation slopes, taken together, indicate that the increased upwelling in the tropics after the year 2000 appears to have triggered an intensification of tracer transport from the tropics into the extratropics in the lower stratosphere below about 500 K. This finding is corroborated by the fact that transit times along the shallow branch of the residual circulation into the LMS have decreased for the same time period (1993–2003). On a longer time scale (1979–2009), the transit time of the shallow residual circulation branch show a steady decrease of about −1 month/decade over the last 30 yr, while the transit times of the deep branch remain unchanged. This highlights that changes in the upwelling across the tropical tropopause are not sufficient as an indicator for changes in the entire Brewer-Dobson circulation.


2008 ◽  
Vol 25 (5) ◽  
pp. 656-666 ◽  
Author(s):  
Herman G. J. Smit ◽  
Andreas Volz-Thomas ◽  
Manfred Helten ◽  
Werner Paetz ◽  
Dieter Kley

Abstract A new in-flight calibration (IFC) method is described for the humidity sensor flown routinely since 1994 on the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program’s aircraft. The IFC method corrects the potential drift of the sensor offset at zero relative humidity, which is the critical parameter in determining the uncertainty of the measurements. The sensor offset is determined from the measurements themselves as obtained during periods when the aircraft is flying in the lower stratosphere at or above the hygropause, where the H2O mixing ratio reaches well-defined minimum values of about 5 ppmv and the contribution of atmospheric H2O to the sensor signal is minimal. The selection of stratospheric data is achieved with the help of potential temperature, which can be calculated in situ from measured temperature and pressure. The IFC method is capable of providing humidity measurements in near–real time with an uncertainty of ±8% RH at the surface and ±7% RH in the upper troposphere. For validation, the IFC method was applied to 5 yr of archived raw signals from the MOZAIC aircraft. The resulting humidity data are in good agreement (within 2% RH) with the original MOZAIC data that used monthly pre- and postflight calibrations of the sensor. The standard deviation of the differences varies with altitude between ±4% and ±6% RH, which is comparable to the accuracy of the MOZAIC laboratory calibrations. Compared to MOZAIC operation based on monthly calibrations in the laboratory, the use of IFC will substantially reduce the efforts for maintenance and thus will enable operation of the sensor on a large fleet of in-service aircraft for near-real-time measurements of humidity in the troposphere. Because the IFC method will not work on aircraft that never enter the lower stratosphere, for example, aircraft that fly exclusively regional routes or in the tropics, regular offline calibrations will remain important for such aircraft.


Author(s):  
Sergey M. Khaykin ◽  
Jean-Pierre Pommereau ◽  
Emmanuel D. Riviere ◽  
Gerhard Held ◽  
Felix Ploeger ◽  
...  

High-resolution in situ balloon measurements of water vapour, aerosol, methane and temperature in the upper Tropical Tropopause Layer (TTL) and lower stratosphere are used to evaluate the processes controlling the stratospheric water budget: horizontal transport (inmixing) and hydration by cross-tropopause overshooting updrafts. The obtained in situ evidences of these phenomena are analyzed using satellite observations by Aura MLS (Microwave Limb Sounder) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) together with trajectory and transport modeling performed using CLaMS (Chemical Lagrangian Model of the Stratosphere) and HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) model. <br><br> Balloon soundings were conducted during March 2012 in Bauru, Brazil (22.3°&thinsp;S) in the frame of the TRO-Pico campaign for studying the impact of convective overshooting on the stratospheric water budget. The balloon payloads included two stratospheric hygrometers: FLASH-B (Fluorescence Lyman-Alpha Stratospheric Hygrometer for Balloon) and Pico-SDLA instrument as well as COBALD (Compact Optical Backscatter Aerosol Detector) sondes, complemented by Vaisala RS-92 radiosondes. Water vapour vertical profiles obtained independently by the two stratospheric hygrometers are in excellent agreement, ensuring credibility of the vertical structures observed. <br><br> A signature of in-mixing is inferred from a series of vertical profiles, showing coincident enhancements in water vapour and aerosol at the 425&thinsp;K (18.5&thinsp;km) level. Trajectory analysis unambiguously links these features to intrusions from the Southern Hemisphere extra-tropical stratosphere, containing more water and aerosol, as demonstrated by MLS and CALIPSO global observations. The in-mixing is successfully reproduced by CLaMS simulations, showing a relatively moist filament extending to 20&thinsp;S°. A signature of local cross-tropopause transport of water is observed in a particular sounding, performed on a convective day and revealing water vapour enhancements of up to 0.6&thinsp;ppmv as high as the 404&thinsp;K (17.8&thinsp;km) level. These are shown to originate from convective overshoots upwind detected by an S-band weather radar operating locally in Bauru. <br><br> The accurate in situ observations uncover two independent moisture pathways into the tropical lower stratosphere, whose manifestations are hardly detectable by space-borne sounders. We argue that the moistening by horizontal transport is limited by the weak meridional gradients of water, whereas the fast convective cross-tropopause transport, largely missed by global models, can have a substantial effect, at least at a regional scale.


2009 ◽  
Vol 9 (6) ◽  
pp. 25049-25084 ◽  
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 analyze the data obtained during five local flights to study the dominant transport processes controlling the tropical tropopause layer (TTL) above West-Africa: deep convection up to the level of main convective outflow, overshooting of deep convection, horizontal inmixing across the subtropical tropopause, and horizontal transport across the subtropical barrier. Except for the flight of 13 August, distinct minima in CO2 indicate convective outflow of boundary layer air in the TTL. The CO2 profiles show that the level of main convective outflow was mostly located 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. 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 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, increasing above this level to 0.2±0.15 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 and 25° N latitude where isentropic mixing between these two regions may occur.


2007 ◽  
Vol 7 (13) ◽  
pp. 3399-3409 ◽  
Author(s):  
T. Christensen ◽  
B. M. Knudsen ◽  
J.-P. Pommereau ◽  
G. Letrenne ◽  
A. Hertzog ◽  
...  

Abstract. The temperature and wind of the ECMWF ERA-40 reanalysis in the tropical lower stratosphere during the period 1988–2001 has been evaluated by comparison with independent in situ measurements of 21 IR Montgolfier and superpressure long-duration balloon flights performed by CNES from Pretoria (26° S) in South Africa in 1988–1989, Latacunga (1° S) in Ecuador in 1991–1998 and Bauru (22° S) in Brazil in 2000–2001. The ERA-40 temperature displays a bias varying progressively from +1.16 K in 1988–1989, to +0.26 K in 1994–1996 and −0.46 K after 1998, the latter being fully consistent with recent evaluations of ECMWF operational analysis from radio occultation and in situ long-duration balloon observations. The amplitude of the bias and its evolution are very similar to the results of a previous evaluation from radiosondes in 1991–2003, suggesting that the origin of the drift of ERA-40 might be mainly due to errors in the series of satellite measurements of MSU, replaced by AMSU in 1998, assimilated in the model. The ERA-40 zonal wind speed in the lower stratosphere appears slightly overestimated by 0.7–1.0 m/s on average in both the tropics and equatorial region, that is by 5–10% compared to the average 10–20 m/s wind speed. This bias, fully consistent with a recent evaluation of ECMWF operational analysis in 2004, is found constant during the whole 1988–2001 period, suggesting a shortfall in the variabililty of ERA-40 horizontal winds in the lower stratosphere in the tropics and the equatorial region. Finally calculated trajectories using ERA-40, frequently used for analysing field observations, are found in error compared to that of the balloons by ±500 km after 5 days and ±1000 km after 10 days.


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