scholarly journals Ice supersaturations exceeding 100% at the cold tropical tropopause: implications for cirrus formation and dehydration

2004 ◽  
Vol 4 (6) ◽  
pp. 7433-7462
Author(s):  
E. Jensen ◽  
J. B. Smith ◽  
L. Pfister ◽  
J. V. Pitman ◽  
E. M. Weinstock ◽  
...  
Keyword(s):  
Water Saturation ◽  
Accommodation Coefficient ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
High Threshold ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
Accommodation Coefficients ◽  
The Tropics

Abstract. Recent in situ measurements at tropical tropopause temperatures as low as 187 K indicate supersaturations with respect to ice exceeding 100% with little or no ice present. In contrast, models used to simulate cloud formation near the tropopause assume a supersaturation threshold for ice nucleation of about 65% based on laboratory measurements of sulfate aerosol freezing. The high supersaturations reported here, along with cloud simulations assuming a plausible range of temperature histories in the sampled air mass, indicate that the vast majority of aerosols in the air sampled on this flight must have had supersaturation thresholds for ice nucleation exceeding 100% (i.e. near liquid water saturation at these temperatures). Possible explanations for this high threshold are that (1) the expressions used for calculating vapor pressure over supercooled water at low temperatures give values at least 20% too low, (2) most of the available aerosols had a composition that makes them much more resistant to ice nucleation than aerosols used in laboratory experiments, and (3) organic films on the aerosol surfaces reduce their accommodation coefficient for uptake of water, resulting in aerosols with more concentrated solutions when moderate-rapid cooling occurs and correspondingly inhibited homogeneous freezing. Simulations of in situ cloud formation in the tropical tropopause layer (TTL) throughout the tropics indicate that if these decreased accommodation coefficients and resulting high thresholds for ice nucleation prevailed throughout the tropics, then the calculated occurrence frequency and areal coverage of TTL cirrus would be significantly suppressed. However, the simulations also show that even if in situ TTL cirrus form only over a very small fraction of the tropics in the western Pacific, enough air passes through them due to rapid horizontal transport such that they can still effectively freeze-dry air entering the stratosphere.

scholarly journals Ice supersaturations exceeding 100% at the cold tropical tropopause: implications for cirrus formation and dehydration

2005 ◽  
Vol 5 (3) ◽  
pp. 851-862 ◽  
Author(s):  
E. J. Jensen ◽  
J. B. Smith ◽  
L. Pfister ◽  
J. V. Pittman ◽  
E. M. Weinstock ◽  
...  
Keyword(s):  
Water Saturation ◽  
Accommodation Coefficient ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
High Threshold ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
Accommodation Coefficients ◽  
The Tropics

Abstract. Recent in situ measurements at tropical tropopause temperatures as low as 187 K indicate supersaturations with respect to ice exceeding 100% with little or no ice present. In contrast, models used to simulate cloud formation near the tropopause assume a supersaturation threshold for ice nucleation of about 65% based on laboratory measurements of aqueous aerosol freezing. The high supersaturations reported here, along with cloud simulations assuming a plausible range of temperature histories in the sampled air mass, indicate that the vast majority of aerosols in the air sampled on this flight must have had supersaturation thresholds for ice nucleation exceeding 100% (i.e. near liquid water saturation at these temperatures). Possible explanations for this high threshold are that (1) the expressions used for calculating vapor pressure over supercooled water at low temperatures give values are at least 20% too low, (2) organic films on the aerosol surfaces reduce their accommodation coefficient for uptake of water, resulting in aerosols with more concentrated solutions when moderate-rapid cooling occurs and correspondingly inhibited homogeneous freezing, and (3) if surface freezing dominates, organic coatings may increase the surface energy of the ice embryo/vapor interface resulting in suppressed ice nucleation. Simulations of in situ cloud formation in the tropical tropopause layer (TTL) throughout the tropics indicate that if decreased accommodation coefficients and resulting high thresholds for ice nucleation prevailed throughout the tropics, then the calculated occurrence frequency and areal coverage of TTL cirrus would be significantly suppressed. However, the simulations also show that even if in situ TTL cirrus form only over a very small fraction of the tropics in the western Pacific, enough air passes through them due to rapid horizontal transport such that they can still effectively freeze-dry air entering the stratosphere. The TTL cirrus simulations show that even if very large supersaturations are required for ice nucleation, these large supersaturations should occur very rarely.

scholarly journals Tracer measurements in the tropical tropopause layer during the AMMA/SCOUT-O3 aircraft campaign

2010 ◽  
Vol 10 (8) ◽  
pp. 3615-3627 ◽  
Author(s):  
C. D. Homan ◽  
C. M. Volk ◽  
A. C. Kuhn ◽  
A. Werner ◽  
J. Baehr ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Deep Convection ◽  
Transport Processes ◽  
Gradual Transition ◽  
Tropical Tropopause Layer ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
Multidisciplinary Analysis ◽  
The Tropics

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.

scholarly journals Tracer measurements in the tropical tropopause layer during the AMMA/SCOUT-O3 aircraft campaign

2009 ◽  
Vol 9 (6) ◽  
pp. 25049-25084 ◽  
Author(s):  
C. D. Homan ◽  
C. M. Volk ◽  
A. C. Kuhn ◽  
A. Werner ◽  
J. Baehr ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Deep Convection ◽  
Transport Processes ◽  
Gradual Transition ◽  
Tropical Tropopause Layer ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
Multidisciplinary Analysis ◽  
The Tropics

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.

scholarly journals More evidence for very short-lived substance contribution to stratospheric chlorine inferred from HCl balloon-borne in situ measurements in the tropics

2010 ◽  
Vol 10 (2) ◽  
pp. 397-409 ◽  
Author(s):  
Y. Mébarki ◽  
V. Catoire ◽  
N. Huret ◽  
G. Berthet ◽  
C. Robert ◽  
...  
Keyword(s):  
In Situ Measurements ◽  
Tunable Diode Laser ◽  
Vertical Profiles ◽  
Tropical Tropopause Layer ◽  
Laser Absorption ◽  
Tropical Tropopause ◽  
Product Gas ◽  
Gas Measurements ◽  
The Tropics

Abstract. Volume mixing ratio (vmr) vertical profiles of hydrogen chloride (HCl) are retrieved from in situ measurements performed by a balloon-borne infrared tunable diode laser absorption spectrometer (SPIRALE) during two balloon flights in the tropics (Teresina, Brazil, 5.1° S–42.9° W) in June 2005 and June 2008. HCl vertical profiles obtained from 15 to 31 km are presented and analysed to estimate the contribution of very short-lived substances (VSLS) to total stratospheric chlorine. Both retrieved vertical profiles of HCl from these flights agree very well with each other, with estimated overall uncertainties of 6% on vmr between 23 and 31 km. Upper limits of HCl vmr as low as 20 pptv in June 2008 and 30 pptv in June 2005 are inferred in the upper part of the tropical tropopause layer (TTL). Backward trajectory calculations and such low amounts suggest that the air masses sampled correspond to typical background conditions, i.e. neither influenced by recent tropospheric nor stratospheric air. Taking into account the recently reported VSL source gas measurements obtained in similar conditions (Laube et al., 2008) and the main intermediate degradation product gas COCl2 (Fu et al., 2007), a total VSLS contribution of 85±40 pptv to stratospheric chlorine is inferred. This refines the WMO (2007) estimation of 50 to 100 pptv, which was not taking into account any HCl contribution. In addition, comparisons of HCl measurements between SPIRALE and the Aura MLS satellite instrument in the tropical lower and middle stratosphere lead to a very good agreement. The previous agreement between MLS-deduced upper stratospheric total chlorine content and modelled values including 100 pptv of VSLS (Froidevaux et al., 2006) is thus supported by our present result about the VSLS contribution.

scholarly journals Influence of gravity wave temperature anomalies and their vertical gradients on cirrus clouds in the tropical tropopause layer – a satellite-based view

2020 ◽  
Vol 20 (21) ◽  
pp. 12499-12514
Author(s):  
Kai-Wei Chang ◽  
Tristan L'Ecuyer
Keyword(s):  
Gravity Wave ◽  
Gravity Waves ◽  
Radio Occultation ◽  
Negative Temperature ◽  
Cloud Formation ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
The Mean ◽  
The Tropics

Abstract. Negative temperature perturbations (T′) from gravity waves are known to be favorable to tropical tropopause layer (TTL) clouds, and recent studies have further suggested a possible role of dT′/dz in facilitating TTL cloud formation and maintenance. With a focus on exploring the influence of dT′/dz on TTL clouds, this study utilizes radio occultation temperature retrievals and cloud layers from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) to understand how gravity wave perturbations modulate cloud occurrence in the tropics. Cloud populations were evaluated in four phases corresponding to positive or negative T′ and dT′/dz. We find that 55 % of TTL clouds are found where T′ and dT′/dz are both negative. Regions of frequent convection are associated with higher cloud populations in the warm phase T′>0. We show that the partitioning of cloud population among wave phases exhibits dependence on background relative humidity. In the phase where T′ and dT′/dz are both negative, the mean cloud effective radius is the smallest of all four phases, but the differences are small. It is shown that the strongest mean negative T′ anomaly is centered on the cloud top, resulting in positive dT′/dz above the cloud top and negative dT′/dz below. This negative T′ anomaly propagates downward with time, characteristic of upward propagating gravity waves. Negative (positive) T′ anomalies are associated with increased (decreased) probability of being occupied by clouds. The magnitude of T′ correlates with the increase or decrease in cloud occurrence, giving evidence that the wave amplitude influences the probability of cloud occurrence. While the decrease in cloud occurrence in the warm phase is centered on the altitude of T′ maxima, we show that the increase in cloud occurrence around T′ minima occurs below the minima in height, indicating that cloud formation or maintenance is facilitated mainly inside negative dT′/dz. Together with existing studies, our results suggest that the cold phase of gravity waves is favorable to TTL clouds mainly through the region where dT′/dz is negative.

scholarly journals Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus

2009 ◽  
Vol 9 (5) ◽  
pp. 20631-20675 ◽  
Author(s):  
E. J. Jensen ◽  
L. Pfister ◽  
T.-P. Bui ◽  
P. Lawson ◽  
D. Baumgardner
Keyword(s):  
Ice Nucleation ◽  
Nucleation Theory ◽  
Ice Crystal ◽  
Tropical Tropopause Layer ◽  
Microphysical Properties ◽  
Tropical Tropopause ◽  
Ice Nuclei ◽  
Ice Crystal Size ◽  
Homogeneous Freezing

Abstract. In past modeling studies, it has generally been assumed that the predominant mechanism for nucleation of ice in the uppermost troposphere is homogeneous freezing of aqueous aerosols. However, recent in situ and remote-sensing measurements of the properties of cirrus clouds at very low temperatures in the tropical tropopause layer (TTL) are broadly inconsistent with theoretial predictions based on the homogeneous freezing assumption. The nearly ubiquitous occurence of gravity waves in the TTL makes the predictions from homogeneous nucleation theory particularly difficult to reconcile with measurements. These measured properties include ice number concentrations, which are much lower than theory predicts; ice crystal size distributions, which are much broader than theory predicts; and cloud extinctions, which are much lower than theory predicts. Although other explanations are possible, one way to limit ice concentrations is to have on the order of 50 L−1 effective ice nuclei (IN) that could nucleate ice at relatively low supersaturations. We suggest that ammonium sulfate particles, which would be dry much of the time in the cold TTL, are a potential IN candidate for TTL cirrus. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.

scholarly journals New investigations on homogeneous ice nucleation: the effects of water activity and water saturation formulations

2022 ◽  
Vol 22 (1) ◽  
pp. 65-91
Author(s):  
Manuel Baumgartner ◽  
Christian Rolf ◽  
Jens-Uwe Grooß ◽  
Julia Schneider ◽  
Tobias Schorr ◽  
...  
Keyword(s):  
Water Activity ◽  
Low Temperatures ◽  
Water Saturation ◽  
Aerosol Particles ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Microphysics Scheme ◽  
Cold Temperatures ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause

Abstract. Laboratory measurements at the AIDA cloud chamber and airborne in situ observations suggest that the homogeneous freezing thresholds at low temperatures are possibly higher than expected from the so-called “Koop line”. This finding is of importance, because the ice onset relative humidity affects the cirrus cloud coverage and, at the very low temperatures of the tropical tropopause layer, together with the number of ice crystals also the transport of water vapor into the stratosphere. Both the appearance of cirrus clouds and the amount of stratospheric water feed back to the radiative budget of the atmosphere. In order to explore the enhanced ice onset humidities, we re-examine the entire homogeneous ice nucleation process, ice onset, and nucleated crystal numbers, by means of a two-moment microphysics scheme embedded in the trajectory-based model (CLaMS-Ice) as follows: the well-understood and described theoretical framework of homogeneous ice nucleation includes certain formulations of the water activity of the freezing aerosol particles and the saturation vapor pressure of water with respect to liquid water. However, different formulations are available for both parameters. Here, we present extensive sensitivity simulations testing the influence of three different formulations for the water activity and four for the water saturation on homogeneous ice nucleation. We found that the number of nucleated ice crystals is almost independent of these formulations but is instead sensitive to the size distribution of the freezing aerosol particles. The ice onset humidities, also depending on the particle size, are however significantly affected by the choices of the water activity and water saturation, in particular at cold temperatures ≲205 K. From the CLaMS-Ice sensitivity simulations, we here provide combinations of water saturation and water activity formulations suitable to reproduce the new, enhanced freezing line.

scholarly journals New investigations on homogeneous ice nucleation: the effects of water activity and water saturation formulations

2021 ◽  
Author(s):  
Manuel Baumgartner ◽  
Christian Rolf ◽  
Jens-Uwe Grooß ◽  
Julia Schneider ◽  
Tobias Schorr ◽  
...  
Keyword(s):  
Water Activity ◽  
Low Temperatures ◽  
Water Saturation ◽  
Aerosol Particles ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Microphysics Scheme ◽  
Cold Temperatures ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause

Abstract. Laboratory measurements at the AIDA cloud chamber and airborne in-situ observations suggest that the homogeneous freezing thresholds at low temperatures are possibly higher than expected from the so-called “Koop-line”. This finding is of importance, because the ice onset relative humidity affects the cirrus cloud coverage and, at the very low temperatures of the tropical tropopause layer, together with the number of ice crystals also the transport of water vapor into the stratosphere. Both, the appearance of cirrus clouds and the amount of stratospheric water feed back to the radiative budget of the atmosphere. In order to explore the enhanced ice onset humidities, we re-examine the entire homogeneous ice nucleation process, ice onset and nucleated crystal numbers, by means of a two-moment microphysics scheme embedded in the trajectory based model (CLaMS-Ice) as follows: the well-understood and described theoretical framework of homogeneous ice nucleation yet includes certain formulations of the water activity of the freezing aerosol particles and the saturation vapor pressure of water with respect to liquid water. However, different formulations are available for both parameters. Here, we present extensive sensitivity simulations testing the influence of three different formulations for the water activity and four for the water saturation on homogeneous ice nucleation. We found that the number of nucleated ice crystals is almost independent of these formulations but is instead sensitive to the size distribution of the freezing aerosol particles. The ice onset humidities, also depending on the particle size, are however significantly affected by the choices of the water activity and water saturation, in particular at cold temperatures  205 K. From the CLaMS-Ice sensitivity simulations, we here provide combinations of water saturation and water activity formulations suitable to reproduce the new, enhanced freezing line.

scholarly journals More evidence for very short-lived substance contribution to stratospheric chlorine inferred from HCl balloon-borne in situ measurements in the tropics

2009 ◽  
Vol 9 (4) ◽  
pp. 16163-16195
Author(s):  
Y. Mébarki ◽  
V. Catoire ◽  
G. Berthet ◽  
N. Huret ◽  
C. Robert
Keyword(s):  
In Situ Measurements ◽  
Tunable Diode Laser ◽  
Vertical Profiles ◽  
Tropical Tropopause Layer ◽  
Laser Absorption ◽  
Tropical Tropopause ◽  
Product Gas ◽  
Gas Measurements ◽  
The Tropics

Abstract. Volume mixing ratio (vmr) vertical profiles of hydrogen chloride (HCl) are retrieved from in situ measurements performed by a balloon-borne infrared tunable diode laser absorption spectrometer (SPIRALE) during two balloon flights in the tropics (Teresina, Brazil, 5.1° S–42.9° W) at three year interval in June 2005 and June 2008. HCl vertical profiles obtained from 15.0 to 31.0 km are presented and analysed to estimate the contribution of very short-lived substances (VSLS) to total stratospheric chlorine. Both retrieved vertical profiles of HCl from these flights globally agree very well with each other, with estimated overall uncertainties of 6% on vmr between 23 and 31 km. Upper limits of HCl vmr as low as (20±20) pptv in June 2008 and (30±30) pptv in June 2005 are inferred in the upper part of the tropical tropopause layer (TTL). Backward trajectory calculations suggest that these low amounts were sampled in air masses corresponding to typical background conditions, i.e. neither influenced by recent tropospheric nor stratospheric air. Taking into account the recently reported VSLS source gas measurements obtained in similar conditions (Laube et al., 2008) and the main intermediate product gas (COCl2), a VSLS contribution of about (85±35 pptv) to total stratospheric chlorine is inferred. This refines the WMO (2007) estimation of 50 to 100 pptv, which was not taking into account any HCl contribution. In addition, comparisons of HCl measurements between SPIRALE and MLS-Aura satellite instrument in the tropical lower and middle stratosphere lead to a very good agreement. Since HCl modelled values derived from a total stratospheric chlorine budget including 100 pptv of VSLS agree with MLS measurements in the upper stratosphere, the consistency between SPIRALE and MLS measurements provides another evidence for this VSLS contribution.

scholarly journals In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 1: Summary of StratoClim results

2021 ◽  
Vol 21 (15) ◽  
pp. 11689-11722
Author(s):  
Ralf Weigel ◽  
Christoph Mahnke ◽  
Manuel Baumgartner ◽  
Antonis Dragoneas ◽  
Bärbel Vogel ◽  
...  
Keyword(s):  
Asian Monsoon ◽  
Particle Formation ◽  
In Situ Observation ◽  
Aerosol Layer ◽  
New Particle Formation ◽  
Tropical Tropopause Layer ◽  
Temperature Anomalies ◽  
Nucleation Mode ◽  
Tropical Tropopause

Abstract. During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal, with eight mission flights of the M-55 Geophysica in the upper troposphere–lower stratosphere (UTLS) of the Asian monsoon anticyclone (AMA) over northern India, Nepal, and Bangladesh. More than 100 events of new particle formation (NPF) were observed. In total, more than 2 h of flight time was spent under NPF conditions as indicated by the abundant presence of nucleation-mode aerosols, i.e. with particle diameters dp smaller than 15 nm, which were detected in situ by means of condensation nuclei counting techniques. Mixing ratios of nucleation-mode particles (nnm) of up to ∼ 50 000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ∼ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause. Resulting nnm remained elevated (∼ 300–2000 mg−1) up to altitudes of ∼ 17.5 km (θ ≈ 400 K), while under NPF conditions the fraction (f) of sub-micrometre-sized non-volatile residues (dp > 10 nm) remained below 50 %. At ∼ 12–14 km (θ ≈ 355–365 K) the minimum of f (< 15 %) was found, and underneath, the median f generally remains below 25 %. The persistence of particles at nucleation-mode sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. The frequency of NPF events observed during StratoClim 2017 underlines the importance of the AMA as a source region for UTLS aerosols and for the formation and maintenance of the Asian tropopause aerosol layer (ATAL). The observed abundance of NPF-produced nucleation-mode particles within the AMA is not unambiguously attributable to (a) specific source regions in the boundary layer (according to backward trajectory analyses), or (b) the direct supply with precursor material by convective updraught (from correlations of NPF with carbon monoxide), or (c) the recent release of NPF-capable material from the convective outflow (according to air mass transport times in the tropical tropopause layer, TTL). Temperature anomalies with ΔT of 2 K (peak-to-peak amplitude), as observed at a horizontal wavelength of ∼ 70–100 km during a level flight of several hours, match with NPF detections and represent an additional mechanism for local increases in supersaturation of the NPF precursors. Effective precursor supply and widely distributed temperature anomalies within the AMA can explain the higher frequency of intense NPF observed during StratoClim 2017 than all previous NPF detections with COPAS (COndensation PArticle counting System) at TTL levels over Brazil, northern Australia, or West Africa.

Sign in / Sign up

Export Citation Format

Share Document