scholarly journals Estimating the contribution of bromoform to stratospheric bromine and its relation to dehydration in the tropical tropopause layer

2006 ◽  
Vol 6 (12) ◽  
pp. 4755-4761 ◽  
Author(s):  
B.-M. Sinnhuber ◽  
I. Folkins

Abstract. The contribution of bromoform to the stratospheric bromine loading is estimated using the one-dimensional tropical mean model of Folkins and Martin (2005), which is constrained by observed mean profiles of temperature and humidity. In order to reach the stratosphere, bromoform needs to be lifted by deep convection into the tropical tropopause layer (TTL), above the level of zero radiative heating. The contribution of bromoform to stratospheric bromine then depends critically on the rate of removal of the degradation products of bromoform (collectively called Bry here) from the TTL, which is believed to be due to scavenging by falling ice. This relates the transport of short-lived bromine species into the stratosphere to processes of dehydration in the TTL. In the extreme case of dehydration occurring only through overshooting deep convection, the loss of Bry from the TTL may be negligible and consequently bromoform will fully contribute with its boundary layer mixing ratio to the stratospheric bromine loading, i.e. with 3 pptv for an assumed 1 pptv of bromoform in the boundary layer. For the other extreme that Bry is removed from the TTL almost instantaneously, the model calculations predict a contribution of about 0.5 pptv for the assumed 1 pptv of boundary layer bromoform. While this gives some constraints on the contribution of bromoform to stratospheric bromine, a key uncertainty in estimating the contribution of short-lived bromine source gases to the stratospheric bromine loading is the mechanism and rate of removal of Bry within the TTL.

2005 ◽  
Vol 5 (6) ◽  
pp. 12939-12956 ◽  
Author(s):  
B.-M. Sinnhuber ◽  
I. Folkins

Abstract. The contribution of bromoform to the stratospheric bromine loading is estimated using the one-dimensional tropical mean model of Folkins and Martin (2005), which is constrained by observed mean profiles of temperature and humidity. In order to reach the stratosphere, bromoform needs to be lifted by deep convection into the tropical tropopause layer (TTL), above the level of zero radiative heating. The contribution of bromoform to stratospheric bromine depends then critically on the rate of removal of the degradation products of bromoform (collectively called Bry here) from the TTL, which is believed to be due to scavenging by falling ice. This relates the transport of short-lived bromine species into the stratosphere to processes of dehydration in the TTL. In the extreme case of dehydration occurring only through overshooting deep convection, the loss of Bry from the TTL may be negligible and consequently bromoform will fully contribute with its boundary layer mixing ratio to the stratospheric bromine loading, i.e. with 3 pptv for an assumed 1 pptv of bromoform in the boundary layer. For the other extreme that Bry is removed from the TTL almost instantaneously, the model calculations predict a contribution of about 0.5 pptv for the assumed 1 pptv of boundary layer bromoform. While this gives some constraints on the contribution of bromoform to stratospheric bromine, it is argued that a more precise number cannot be given until the mechanisms of dehydration in the TTL are better understood.


2014 ◽  
Vol 14 (11) ◽  
pp. 5781-5792 ◽  
Author(s):  
Q. Liang ◽  
E. Atlas ◽  
D. Blake ◽  
M. Dorf ◽  
K. Pfeilsticker ◽  
...  

Abstract. We use the NASA Goddard Earth Observing System (GEOS) Chemistry Climate Model (GEOSCCM) to quantify the contribution of the two most important brominated very short lived substances (VSLSs), bromoform (CHBr3) and dibromomethane (CH2Br2), to stratospheric bromine and its sensitivity to convection strength. Model simulations suggest that the most active transport of VSLSs from the marine boundary layer through the tropopause occurs over the tropical Indian Ocean, the tropical western Pacific, and off the Pacific coast of Mexico. Together, convective lofting of CHBr3 and CH2Br2 and their degradation products supplies ~8 ppt total bromine to the base of the tropical tropopause layer (TTL, ~150 hPa), similar to the amount of VSLS organic bromine available in the marine boundary layer (~7.8–8.4 ppt) in the active convective lofting regions mentioned above. Of the total ~8 ppt VSLS bromine that enters the base of the TTL at ~150 hPa, half is in the form of organic source gases and half in the form of inorganic product gases. Only a small portion (<10%) of the VSLS-originated bromine is removed via wet scavenging in the TTL before reaching the lower stratosphere. On average, globally, CHBr3 and CH2Br2 together contribute ~7.7 pptv to the present-day inorganic bromine in the stratosphere. However, varying model deep-convection strength between maximum (strongest) and minimum (weakest) convection conditions can introduce a ~2.6 pptv uncertainty in the contribution of VSLSs to inorganic bromine in the stratosphere (BryVSLS). Contrary to conventional wisdom, the minimum convection condition leads to a larger BryVSLS as the reduced scavenging in soluble product gases, and thus a significant increase in product gas injection (2–3 ppt), greatly exceeds the relatively minor decrease in source gas injection (a few 10ths ppt).


2015 ◽  
Vol 15 (12) ◽  
pp. 16655-16696 ◽  
Author(s):  
R. Newton ◽  
G. Vaughan ◽  
H. M. A. Ricketts ◽  
L. L. Pan ◽  
A. J. Weinheimer ◽  
...  

Abstract. We present a series of ozonesonde profiles measured from Manus Island, Papua New Guinea, during February 2014. The experiment formed a part of a wider airborne campaign involving three aircraft based in Guam, to characterise the atmospheric composition above the tropical West Pacific in unprecedented detail. Thirty-nine ozonesondes were launched between 2 and 25 February, of which 34 gave good ozone profiles. Particular attention was paid to measuring the background current of the ozonesonde before launch, as this can amount to half the measured signal in the tropical tropopause layer (TTL). An unexpected contamination event affected these measurements and required a departure from standard operating procedures for the ozonesondes. Comparison with aircraft measurements allows validation of the measured ozone profiles and confirms that for well-characterized sondes (background current <50 nA) a constant background current should be assumed throughout the profile, equal to the minimum value measured during preparation just before launch. From this set of 34 ozonesondes, the minimum reproducible ozone concentration measured in the TTL was 12–13 ppbv; no examples of near-zero ozone concentration as reported by other recent papers were measured. The lowest ozone concentrations coincided with outflow from extensive deep convection to the east of Manus, consistent with uplift of ozone-poor air from the boundary layer. However, these minima were lower than the ozone concentration measured through most of the boundary layer, and were matched only by measurements at the surface in Manus.


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.


2011 ◽  
Vol 11 (8) ◽  
pp. 22199-22245 ◽  
Author(s):  
S. Brinckmann ◽  
A. Engel ◽  
H. Bönisch ◽  
B. Quack ◽  
E. Atlas

Abstract. We conducted measurements of up to the five important short-lived brominated species in the marine boundary layer (MBL) of the mid-latitudes (List/Sylt, North Sea) in June 2009 and of the tropical Western Pacific during the TransBrom ship campaign in October 2009. For the one-week time series in List mean mixing ratios of 2.0, 1.1, 0.2, 0.1 ppt were analysed for CHBr3, CH2Br2, CHBr2Cl and CH2BrCl, with maxima of 5.8 and 1.6 ppt for the two main components CHBr3 and CH2Br2. Along the cruise track in the Western Pacific (between 41° N and 13° S) mean mixing ratios of 1.0, 0.9, 0.2, 0.1 and 0.1 ppt for CHBr3, CH2Br2, CHBrCl2, CHBr2Cl and CH2BrCl were determined. Air samples with coastal influence showed considerably higher mixing ratios than the samples with open ocean origin. Correlation analyses of the two datasets yielded strong linear relationships between the mixing ratios of four of the five species (except for CH2BrCl). Using a combined dataset from the two campaigns, rough estimates of the molar emission ratios between the correlated substances were derived as follows: 9/1/0.3/0.3 for CHBr3/CH2Br2/CHBrCl2/CHBr2Cl. Additional measurements were made in the tropical tropopause layer (TTL) above Teresina (Brazil, 5.07° S, 42.87° W) in June 2008, using balloon-borne cryogenic whole air sampling technique. Near the level of zero clear-sky net radiative heating (LZRH) at 14.8 km about 2.25 ppt organic bromine was bound to the five short-lived species, making up 13 % of total organic bromine (17.82 ppt). CH2Br2 (1.45 ppt) and CHBr3 (0.56 ppt) accounted for 90 % of the budget of short-lived compounds in that region. Near the tropopause (at 17.5 km) organic bromine from short-lived substances was reduced to 1.35 ppt, with 1.07 ppt and 0.12 ppt attributed to CH2Br2 and CHBr3 respectively.


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.


2011 ◽  
Vol 11 (5) ◽  
pp. 16147-16183 ◽  
Author(s):  
V. Marécal ◽  
G. Krysztofiak ◽  
Y. Mébarki ◽  
V. Catoire ◽  
F. Lott ◽  
...  

Abstract. This paper documents measurements of carbon monoxide (CO), ozone (O3) and temperature in the tropical tropopause layer over Equatorial Brazil for the first time. These measurements were sampled by the balloon-borne instrument SPIRALE (Spectroscopie Infa-Rouge par Absorption de Lasers Embarqués) in June 2005 and in June 2008, both at the transition period from wet to dry season. The height of the Tropical Tropopause Layer (TTL) top and bottom determined from the chemical species profiles are similar for the two flights. Nevertheless the measured profiles of ozone and CO are different in their volume mixing ratio and shape. The larger CO values measured in the TTL in 2005 can be linked to a more intense biomass burning activity in 2005 than in 2008. We also show that both measured profiles are influenced by convection but in different ways leading to different shapes. The CO profile in 2005 is characterised by a generally smooth decrease in the TTL from tropospheric to stratospheric conditions, except for two layers of enhanced CO around 14.2 (>100 parts per billion by volume = ppbv) and 16.3 km altitude (>85 ppbv). Backward trajectories indicate that these layers come from the vertical transport by remote deep convection occurring 2 and 3 days prior to the flight, respectively. This shows that the transition period from wet to dry season is favourable for the transport of significant amounts of CO in the TTL, sometimes above the level of zero radiative heating, because of increasing biomass burning together with decaying but still important convective activity. In 2008 we focus our analysis on a 1 km deep layer, between 17 and 18 km, where both the temperature and the ozone profiles are uniform in the vertical, corresponding to a layer of well-mixed air. We show that this unusual behaviour is indirectly related to the interaction between convection and the Quasi-Biennial Oscillation (QBO), through vertically propagating gravity waves. Quasi-stationary gravity waves are likely to be produced by convective systems and certainly break in the intense wind shear that imposes the QBO at these altitudes. This conclusion is supported by the fact that the 16–18 km layer is devoid of ice particles (hence the mixing is not convective) and from backward trajectories that point towards a convective region as the origin of the air masses in this layer.


2021 ◽  
Vol 21 (20) ◽  
pp. 15493-15518
Author(s):  
Jing Feng ◽  
Yi Huang

Abstract. The tropical tropopause layer (TTL) is the transition layer between the troposphere and the stratosphere. Tropical cyclones may impact the TTL by perturbing the vertical distributions of cloud, temperature, and water vapor. This study combines several A-Train instruments, including radar from CloudSat, lidar from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, and the Atmospheric Infrared Sounder (AIRS) on the Aqua satellite, to detect signatures of cyclone impacts on the distribution patterns of cloud, water vapor, temperature, and radiation by compositing these thermodynamic fields relative to the cyclone center location. Based on the CloudSat 2B-CLDCLASS-LIDAR product, this study finds that tropical cyclone events considerably increase the occurrence frequencies of TTL clouds, in the form of cirrus clouds above a clear troposphere. The amount of TTL cloud ice, however, is found to be mostly contributed by overshooting deep convection that penetrates the base of the TTL at 16 km. To overcome the lack of temperature and water vapor products in cloudy conditions, this study implements a synergistic method that retrieves temperature, water vapor, ice water content, and effective radius simultaneously by incorporating observations from AIRS, CloudSat, and CALIPSO. Using the synergistic method, we find a vertically oscillating pattern of temperature anomalies above tropical cyclones, with warming beneath the cloud top (around 16 km) and cooling above. Based on water vapor profiles retrieved by the synergistic method, we find that the layer integrated water vapor (LIWV) above 16 km is higher above tropical cyclones, especially above overshooting deep convective clouds, compared to climatological values. Moreover, we find that the longwave and net radiative cooling effect of clouds prevails within 1000 km of tropical cyclone centers. The radiative heating effects of clouds from the CloudSat 2B-FLXHR-LIDAR product are well differentiated by the collocated brightness temperature of an infrared window channel from the collocated AIRS L1B product. By performing instantaneous radiative heating rate calculations, we further find that TTL hydration is usually associated with radiative cooling of the TTL, which inhibits the diabatic ascent of moist air across isentropic surfaces to the stratosphere. Therefore, the radiative balance of the TTL under the impact of the cyclone does not favor the maintenance of moist anomalies in the TTL or transporting water vertically to the stratosphere.


2014 ◽  
Vol 14 (1) ◽  
pp. 651-676
Author(s):  
Q. Liang ◽  
E. Atlas ◽  
D. Blake ◽  
M. Dorf ◽  
K. Pfeilsticker ◽  
...  

Abstract. We use the NASA GEOS Chemistry Climate Model (GEOSCCM) to quantify the contribution of two most important brominated very short-lived substances (VSLS), bromoform (CHBr3) and dibromomethane (CH2Br2), to stratospheric bromine and its sensitivity to convection strength. Model simulations suggest that the most active transport of VSLS from the marine boundary layer through the tropopause occurs over the tropical Indian Ocean, the Western Pacific warm pool, and off the Pacific coast of Mexico. Together, convective lofting of CHBr3 and CH2Br2 and their degradation products supplies ∼8 ppt total bromine to the base of the Tropical Tropopause Layer (TTL, ∼150 hPa), similar to the amount of VSLS organic bromine available in the marine boundary layer (∼7.8–8.4 ppt) in the above active convective lofting regions. Of the total ∼8 ppt VSLS-originated bromine that enters the base of TTL at ∼150 hPa, half is in the form of source gas injection (SGI) and half as product gas injection (PGI). Only a small portion (< 10%) the VSLS-originated bromine is removed via wet scavenging in the TTL before reaching the lower stratosphere. On global and annual average, CHBr3 and CH2Br2, together, contribute ∼7.7 pptv to the present-day inorganic bromine in the stratosphere. However, varying model deep convection strength between maximum and minimum convection conditions can introduce a ∼2.6 pptv uncertainty in the contribution of VSLS to inorganic bromine in the stratosphere (BryVSLS). Contrary to the conventional wisdom, minimum convection condition leads to a larger BryVSLS as the reduced scavenging in soluble product gases, thus a significant increase in PGI (2–3 ppt), greatly exceeds the relative minor decrease in SGI (a few 10ths ppt).


2018 ◽  
Vol 18 (7) ◽  
pp. 5157-5171 ◽  
Author(s):  
Richard Newton ◽  
Geraint Vaughan ◽  
Eric Hintsa ◽  
Michal T. Filus ◽  
Laura L. Pan ◽  
...  

Abstract. Ozonesondes reaching the tropical tropopause layer (TTL) over the west Pacific have occasionally measured layers of very low ozone concentrations – less than 15 ppbv – raising the question of how prevalent such layers are and how they are formed. In this paper, we examine aircraft measurements from the Airborne Tropical Tropopause Experiment (ATTREX), the Coordinated Airborne Studies in the Tropics (CAST) and the Convective Transport of Active Species in the Tropics (CONTRAST) experiment campaigns based in Guam in January–March 2014 for evidence of very low ozone concentrations and their relation to deep convection. The study builds on results from the ozonesonde campaign conducted from Manus Island, Papua New Guinea, as part of CAST, where ozone concentrations as low as 12 ppbv were observed between 100 and 150 hPa downwind of a deep convective complex. TTL measurements from the Global Hawk unmanned aircraft show a marked contrast between the hemispheres, with mean ozone concentrations in profiles in the Southern Hemisphere between 100 and 150 hPa of between 10.7 and 15.2 ppbv. By contrast, the mean ozone concentrations in profiles in the Northern Hemisphere were always above 15.4 ppbv and normally above 20 ppbv at these altitudes. The CAST and CONTRAST aircraft sampled the atmosphere between the surface and 120 hPa, finding very low ozone concentrations only between the surface and 700 hPa; mixing ratios as low as 7 ppbv were regularly measured in the boundary layer, whereas in the free troposphere above 200 hPa concentrations were generally well in excess of 15 ppbv. These results are consistent with uplift of almost-unmixed boundary-layer air to the TTL in deep convection. An interhemispheric difference was found in the TTL ozone concentrations, with values < 15 ppbv measured extensively in the Southern Hemisphere but seldom in the Northern Hemisphere. This is consistent with a similar contrast in the low-level ozone between the two hemispheres found by previous measurement campaigns. Further evidence of a boundary-layer origin for the uplifted air is provided by the anticorrelation between ozone and halogenated hydrocarbons of marine origin observed by the three aircraft.


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