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

2010 ◽  
Vol 10 (3) ◽  
pp. 1369-1384 ◽  
Author(s):  
E. J. Jensen ◽  
L. Pfister ◽  
T.-P. Bui ◽  
P. Lawson ◽  
D. Baumgardner
Keyword(s):  
Ammonium Sulfate ◽  
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. However, this mechanism remains to be fully quantified for the size distribution of ammonium sulfate (possibly internally mixed with organics) actually present in the upper troposphere. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.

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 Tropical tropopause ice clouds: a dynamic approach to the mystery of low crystal numbers

2013 ◽  
Vol 13 (19) ◽  
pp. 9801-9818 ◽  
Author(s):  
P. Spichtinger ◽  
M. Krämer
Keyword(s):  
Gravity Waves ◽  
Large Scale ◽  
Full Range ◽  
Ice Nucleation ◽  
Ice Formation ◽  
Ice Crystal ◽  
Ice Clouds ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
Homogeneous Freezing

Abstract. The occurrence of high, persistent ice supersaturation inside and outside cold cirrus in the tropical tropopause layer (TTL) remains an enigma that is intensely debated as the "ice supersaturation puzzle". However, it was recently confirmed that observed supersaturations are consistent with very low ice crystal concentrations, which is incompatible with the idea that homogeneous freezing is the major method of ice formation in the TTL. Thus, the tropical tropopause "ice supersaturation puzzle" has become an "ice nucleation puzzle". To explain the low ice crystal concentrations, a number of mainly heterogeneous freezing methods have been proposed. Here, we reproduce in situ measurements of frequencies of occurrence of ice crystal concentrations by extensive model simulations, driven by the special dynamic conditions in the TTL, namely the superposition of slow large-scale updraughts with high-frequency short waves. From the simulations, it follows that the full range of observed ice crystal concentrations can be explained when the model results are composed from scenarios with consecutive heterogeneous and homogeneous ice formation and scenarios with pure homogeneous ice formation occurring in very slow (< 1 cm s−1) and faster (> 1 cm s−1) large-scale updraughts, respectively. This statistical analysis shows that about 80% of TTL cirrus can be explained by "classical" homogeneous ice nucleation, while the remaining 20% stem from heterogeneous and homogeneous freezing occurring within the same environment. The mechanism limiting ice crystal production via homogeneous freezing in an environment full of gravity waves is the shortness of the gravity waves, which stalls freezing events before a higher ice crystal concentration can be formed.

scholarly journals Composition of cirrus-forming aerosols at the tropical tropopause

2009 ◽  
Vol 9 (5) ◽  
pp. 20347-20369 ◽  
Author(s):  
K. D. Froyd ◽  
D. M. Murphy ◽  
P. Lawson ◽  
D. Baumgardner ◽  
R. L. Herman
Keyword(s):  
Organic Aerosols ◽  
Ice Crystals ◽  
Ice Crystal ◽  
Laboratory Studies ◽  
Tropical Tropopause ◽  
Ice Nuclei ◽  
Homogeneous Freezing ◽  
Biomass Burning Particles ◽  
Recent Laboratory ◽  
Probe Measurements

Abstract. The composition of residual particles from evaporated cirrus ice crystals near the tropical tropopause as well as unfrozen aerosols were measured with a single particle mass spectrometer. Subvisible cirrus residuals were predominantly composed of internal mixtures of neutralized sulfate with organic material and were chemically indistinguishable from unfrozen sulfate-organic aerosols. Ice residuals were also similar in size to unfrozen aerosol. Heterogeneous ice nuclei such as mineral dust were not enhanced in these subvisible cirrus residuals. Biomass burning particles were depleted in the residuals. Cloud probe measurements showing low cirrus ice crystal number concentrations were inconsistent with conventional homogeneous freezing. Recent laboratory studies provide heterogeneous nucleation scenarios that may explain tropopause level subvisible cirrus formation.

scholarly journals The origin of midlatitude ice clouds and the resulting influence on their microphysical properties

2015 ◽  
Vol 15 (23) ◽  
pp. 34243-34281 ◽  
Author(s):  
A. E. Luebke ◽  
A. Afchine ◽  
A. Costa ◽  
J. Meyer ◽  
C. Rolf ◽  
...  
Keyword(s):  
Bimodal Distribution ◽  
Cirrus Clouds ◽  
Ice Crystals ◽  
Radiative Properties ◽  
Ice Crystal ◽  
Ice Clouds ◽  
Microphysical Properties ◽  
Ice Crystal Size ◽  
Ice Water

Abstract. The radiative role of ice clouds in the atmosphere is known to be important, but uncertainties remain concerning the magnitude and net effects. However, through measurements of the microphysical properties of cirrus clouds, we can better characterize them, which can ultimately allow for their radiative properties to be more accurately ascertained. It has recently been proposed that there are two types of cirrus clouds – in situ and liquid origin. In this study, we present observational evidence to show that two distinct types of cirrus do exist. Airborne, in situ measurements of cloud ice water content (IWC), ice crystal concentration (Nice), and ice crystal size from the 2014 ML-CIRRUS campaign provide cloud samples that have been divided according to their origin type. The key features that set liquid origin cirrus apart from the in situ origin cirrus are a higher frequency of high IWC (> 100 ppmv), higher Nice values, and larger ice crystals. A vertical distribution of Nice shows that the in situ origin cirrus clouds exhibit a median value of around 0.1 cm−3, while the liquid origin concentrations are slightly, but notably higher. The median sizes of the crystals contributing the most mass are less than 200 μm for in situ origin cirrus, with some of the largest crystals reaching 550 μm in size. The liquid origin cirrus, on the other hand, were observed to have median diameters greater than 200 μm, and crystals that were up to 750 μm. An examination of these characteristics in relation to each other and their relationship to temperature provides strong evidence that these differences arise from the dynamics and conditions in which the ice crystals formed. Additionally, the existence of these two groups in cirrus cloud populations may explain why a bimodal distribution in the IWC-temperature relationship has been observed. We hypothesize that the low IWC mode is the result of in situ origin cirrus and the high IWC mode is the result of liquid origin cirrus.

scholarly journals The origin of midlatitude ice clouds and the resulting influence on their microphysical properties

2016 ◽  
Vol 16 (9) ◽  
pp. 5793-5809 ◽  
Author(s):  
Anna E. Luebke ◽  
Armin Afchine ◽  
Anja Costa ◽  
Jens-Uwe Grooß ◽  
Jessica Meyer ◽  
...  
Keyword(s):  
Bimodal Distribution ◽  
Cirrus Clouds ◽  
Ice Crystals ◽  
Radiative Properties ◽  
Ice Crystal ◽  
Ice Clouds ◽  
Microphysical Properties ◽  
Ice Crystal Size ◽  
Ice Water

Abstract. The radiative role of ice clouds in the atmosphere is known to be important, but uncertainties remain concerning the magnitude and net effects. However, through measurements of the microphysical properties of cirrus clouds, we can better characterize them, which can ultimately allow for their radiative properties to be more accurately ascertained. Recently, two types of cirrus clouds differing by formation mechanism and microphysical properties have been classified – in situ and liquid origin cirrus. In this study, we present observational evidence to show that two distinct types of cirrus do exist. Airborne, in situ measurements of cloud ice water content (IWC), ice crystal concentration (Nice), and ice crystal size from the 2014 ML-CIRRUS campaign provide cloud samples that have been divided according to their origin type. The key features that set liquid origin cirrus apart from the in situ origin cirrus are higher frequencies of high IWC ( > 100 ppmv), higher Nice values, and larger ice crystals. A vertical distribution of Nice shows that the in situ origin cirrus clouds exhibit a median value of around 0.1 cm−3, while the liquid origin concentrations are slightly, but notably higher. The median sizes of the crystals contributing the most mass are less than 200 µm for in situ origin cirrus, with some of the largest crystals reaching 550 µm in size. The liquid origin cirrus, on the other hand, were observed to have median diameters greater than 200 µm, and crystals that were up to 750 µm. An examination of these characteristics in relation to each other and their relationship to temperature provides strong evidence that these differences arise from the dynamics and conditions in which the ice crystals formed. Additionally, the existence of these two groups in cirrus cloud populations may explain why a bimodal distribution in the IWC-temperature relationship has been observed. We hypothesize that the low IWC mode is the result of in situ origin cirrus and the high IWC mode is the result of liquid origin cirrus.

Evidence of in Situ Cirrus Formation in the Tropical Tropopause Layer over the Southwestern Indian Ocean 

2021 ◽  
Author(s):  
Stephanie Evan ◽  
Irene Reinares Martinez ◽  
Frank G. Wienhold ◽  
Jerome Brioude ◽  
Eric J. Jensen ◽  
...  
Keyword(s):  
Indian Ocean ◽  
High Frequency ◽  
Ice Crystals ◽  
Tropical Tropopause Layer ◽  
Optical Modeling ◽  
Tropical Tropopause ◽  
Vertical Wind Speed ◽  
Homogeneous Freezing ◽  
Southwestern Indian Ocean

&lt;p&gt;A nascent in situ cirrus was observed on 11 January 2019 in the tropical tropopause layer (TTL) over the southwestern Indian Ocean, with the use of balloon-borne instruments. Data from CFH (Cryogenic Frost Point Hygrometer) and COBALD (Compact Optical Backscatter and AerosoL Detector) instruments were used to characterize the cirrus and its environment. Optical modeling was employed to estimate the cirrus microphysical&lt;br&gt;properties from the COBALD backscatter measurements. Newly-formed ice crystals with radius &lt;1 &amp;#956;m and concentration &amp;#8764;500 L &lt;sup&gt;&amp;#8722;1&lt;/sup&gt; were reported at the tropopause. The relatively low concentration and CFH ice supersaturation (1.5) suggests a homogeneous freezing event stalled by a high-frequency gravity wave. The observed vertical wind speed and temperature anomalies that triggered the cirrus formation were due to a 1.5-km vertical-&lt;br&gt;scale wave, as shown by a spectral analysis. This cirrus observation shortly after nucleation is beyond remote sensing capabilities and presents a type of cirrus never reported before.&lt;/p&gt;

scholarly journals Tropical tropopause ice clouds: a dynamic approach to the mystery of low crystal numbers

2012 ◽  
Vol 12 (10) ◽  
pp. 28109-28153 ◽  
Author(s):  
P. Spichtinger ◽  
M. Krämer
Keyword(s):  
Gravity Waves ◽  
Large Scale ◽  
Full Range ◽  
Ice Nucleation ◽  
Ice Formation ◽  
Ice Crystal ◽  
Ice Clouds ◽  
Tropical Tropopause Layer ◽  
Tropical Tropopause ◽  
Homogeneous Freezing

Abstract. The occurrence of high, persistent ice supersaturation inside and outside cold cirrus in the tropical tropopause layer (TTL) remains an enigma that is intensely debated as the "ice supersaturation puzzle". However, it was recently confirmed that observed supersaturations are consistent with very low ice crystal concentrations, which is incompatible with the idea that homogeneous freezing is the major method of ice formation in the TTL. Thus, the tropical tropopause "ice supersaturation puzzle" has become an "ice nucleation puzzle". To explain the low ice crystal concentrations, a number of mainly heterogeneous freezing methods have been proposed. Here, we reproduce in situ measurements of frequencies of occurrence of ice crystal concentrations by extensive model simulations, driven by the special dynamic conditions in the TTL, namely the superposition of slow large-scale updraughts with high-frequency short waves. From the simulations, it follows that the full range of observed ice crystal concentrations can be explained when the model results of the scenarios are mixed for both heterogeneous/homogeneous and pure homogeneous ice formation occurring in very slow (<1 cm s−1) and faster (>1 cm s−1) large-scale updraughts. This statistical analysis shows that about 80% of TTL cirrus can be explained by "classical" homogeneous ice nucleation, while the remaining 20% stem from heterogeneous and homogeneous freezing occurring within the same environment. The mechanism limiting ice crystal production via homogeneous freezing in an environment full of gravity waves is the shortness of the gravity waves, which stalls freezing events before a higher ice crystal concentration can be formed.

scholarly journals Aerosols that form subvisible cirrus at the tropical tropopause

2010 ◽  
Vol 10 (1) ◽  
pp. 209-218 ◽  
Author(s):  
K. D. Froyd ◽  
D. M. Murphy ◽  
P. Lawson ◽  
D. Baumgardner ◽  
R. L. Herman
Keyword(s):  
Organic Aerosols ◽  
Ice Crystals ◽  
Ice Crystal ◽  
Laboratory Studies ◽  
Tropical Tropopause ◽  
Ice Nuclei ◽  
Homogeneous Freezing ◽  
Biomass Burning Particles ◽  
Recent Laboratory ◽  
Probe Measurements

Abstract. The composition of residual particles from evaporated cirrus ice crystals near the tropical tropopause as well as unfrozen aerosols were measured with a single particle mass spectrometer. Subvisible cirrus residuals were predominantly composed of internal mixtures of neutralized sulfate with organic material and were chemically indistinguishable from unfrozen sulfate-organic aerosols. Ice residuals were also similar in size to unfrozen aerosol. Heterogeneous ice nuclei such as mineral dust were not enhanced in these subvisible cirrus residuals. Biomass burning particles were depleted in the residuals. Cloud probe measurements showing low cirrus ice crystal number concentrations were inconsistent with conventional homogeneous freezing. Recent laboratory studies provide heterogeneous nucleation scenarios that may explain tropopause level subvisible cirrus formation.

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.

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.

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