Modelling the progression in the mix of particles within the Arctic stratospheric aerosol layer, including the seasonal source of meteoric smoke particles from the Arctic winter polar vortex 

2021 ◽  
Author(s):  
Kamalika Sengupta ◽  
Graham Mann ◽  
Ralf Weigel ◽  
James Brooke ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Particle Concentration ◽  
Aerosol Particles ◽  
Polar Vortex ◽  
Stratospheric Aerosol ◽  
The Arctic ◽  
Smoke Particles ◽  
Meteoric Smoke ◽  
Winter Time

<p>Meteoric smoke particles (MSPs) provide a steady source of condensation nuclei to the Arctic lower stratosphere, with heterogeneous nucleation to sulphuric acid aerosol particles.  Internally mixed meteoric-sulphuric particles likely also play a significant role in the formation of polar stratospheric clouds and thereby influence stratospheric ozone depletion chemistry, particularly in the quiescent stratosphere.</p><p>In several Arctic winter field campaigns (EUPLEX 2002/3, RECONCILE 2009/10, ESSenCe 2010/11),  in-situ stratospheric aerosol particle concentrations measurements were made from the high-altitude Geophysica aircraft, the COPAS instrument measuring total and refractory (non-volatile) particle concentrations at 20 km altitude (see Curtius et al., 2003; Weigel et al., 2014).  </p><p>These measurements are consistent with there being a substantial seasonal source of meteoric-sulphuric particles to the lower Arctic stratosphere, from each year’s influx of MSPs  within the winter-time Arctic polar vortex. In this study we investigate the effect of MSPs on the quiescent Junge layer particle concentration as the polar vortex builds up and after it dissipates. </p><p>We use the nudged configuration of the UM-UKCA stratosphere-troposphere composition-climate model to reproduce the vertical profile of stratospheric particles measured in-situ during the COPAS 2003 campaign. Our model simulates two types of stratospheric aerosol particles - pure sulphuric acid particles and sulphuric acid particles with a MSP-core. We show that the model is able to reproduce the vertical profile of aerosol particles observed during the COPAS measurements in winter 2003.</p><p>Our findings illustrate the influx of MSP and SO2 from higher altitudes through the polar vortex, the winter-time build-up of SO2 triggering homogeneous nucleation of pure sulphuric particles, also with the seasonal source of MSP-core sulphuric particles nucleated heterogeneously. We assess the effects of MSPs on the quiescent period particle concentration in the Arctic during winter through to spring.</p>

scholarly journals Interactions of meteoric smoke particles with sulphuric acid in the Earth's stratosphere

2012 ◽  
Vol 12 (1) ◽  
pp. 1553-1584
Author(s):  
R. W. Saunders ◽  
S. Dhomse ◽  
W. S. Tian ◽  
M. P. Chipperfield ◽  
J. M. C. Plane
Keyword(s):  
Sulphuric Acid ◽  
Climate Model ◽  
Middle Atmosphere ◽  
Magnesium Silicate ◽  
Stratospheric Aerosol ◽  
Solution Viscosity ◽  
Time Resolved ◽  
Optical Extinction ◽  
Smoke Particles ◽  
Meteoric Smoke

Abstract. Nano-sized meteoric smoke particles (MSPs) with iron-magnesium silicate compositions, formed in the upper mesosphere as a result of meteoric ablation, may remove sulphuric acid from the gas-phase above 40 km and may also affect the composition and behaviour of supercooled H2SO4-H2O droplets in the global stratospheric aerosol (Junge) layer. This study describes a time-resolved spectroscopic analysis of the evolution of the ferric (Fe3+) ion originating from amorphous ferrous (Fe2+)-based silicate powders dissolved in varying Wt % sulphuric acid (30–75%) solutions over a temperature range of 223–295 K. Complete dissolution of the particles was observed under all conditions. The first-order rate coefficient for dissolution decreases at higher Wt % and lower temperature, which is consistent with the increased solution viscosity limiting diffusion of H2SO4 to the particle surfaces. Dissolution under stratospheric conditions should take less than a week, and is much faster than the dissolution of crystalline Fe2+ compounds. The chemistry climate model UMSLIMCAT (based on the UKMO Unified Model) was then used to study the transport of MSPs through the middle atmosphere. A series of model experiments were performed with different uptake coefficients. Setting the concentration of 1.5 nm radius MSPs at 80 km to 3000 cm−3 (based on rocket-borne charged particle measurements), the model matches the reported Wt % Fe values of 0.5–1.0 in Junge layer sulphate particles, and the MSP optical extinction between 40 and 75 km measured by a satellite-borne spectrometer, if the global meteoric input rate is about 20 t d−1. The model indicates that an uptake coefficient ≥0.01 is required to account for the observed two orders of magnitude depletion of H2SO4 vapour above 40 km.

The prevalence of meteoric-sulphuric particles within the stratospheric aerosol layer

2021 ◽  
Author(s):  
Graham Mann ◽  
James Brooke ◽  
Kamalika Sengupta ◽  
Lauren Marshall ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
High Latitude ◽  
Climate Model ◽  
Polar Vortex ◽  
Stratospheric Aerosol ◽  
Light Extinction ◽  
The Arctic ◽  
Aerosol Layer ◽  
Aerosol Composition ◽  
Particle Layer

<p>The widespread presence of meteoric smoke particles (MSPs) within a distinct class of stratospheric aerosol particles has become clear from in-situ measurements in the Arctic, Antarctic and at mid-latitudes.<br> <br>We apply an adapted version of the interactive stratosphere aerosol configuration of the composition-climate model UM-UKCA, to predict the global distribution of meteoric-sulphuric particles nucleated heterogeneously on MSP cores. We compare the UM-UKCA results to new MSP-sulphuric simulations with the European stratosphere-troposphere chemistry-aerosol modelling system IFS-CB05-BASCOE-GLOMAP.</p><p><br>The simulations show a strong seasonal cycle in meteoric-sulphuric particle abundance results from the winter-time source of MSPs transported down into the stratosphere in the polar vortex. Coagulation during downward transport sees high latitude MSP concentrations reduce from ~500 per cm3 at 40km to ~20 per cm3 at 25km, the uppermost extent of the stratospheric aerosol particle layer (the Junge layer).<br> <br>Once within the Junge layer's supersaturated environment, meteoric-sulphuric particles form readily on the MSP cores, growing to 50-70nm dry-diameter (Dp) at 20-25km. Further inter-particle coagulation between these non-volatile particles reduces their number to 1-5 per cc at 15-20km, particle sizes there larger, at Dp ~100nm.</p><p><br>The model predicts meteoric-sulphurics in high-latitude winter comprise >90% of Dp>10nm particles above 25km, reducing to ~40% at 20km, and ~10% at 15km.<br> <br>These non-volatile particle fractions are slightly less than measured from high-altitude aircraft in the lowermost Arctic stratosphere (Curtius et al., 2005; Weigel et al., 2014), and consistent with mid-latitude aircraft measurements of lower stratospheric aerosol composition (Murphy et al., 1998), total particle concentrations  also matching in-situ balloon measurements from Wyoming (Campbell and Deshler, 2014).<br> <br>The MSP-sulphuric interactions also improve agreement with SAGE-II observed stratospheric aerosol extinction in the quiescent 1998-2002 period. <br> <br>Simulations with a factor-8-elevated MSP input form more Dp>10nm meteoric-sulphurics, but the increased number sees fewer growing to Dp ~100nm, the increased MSPs reducing the stratospheric aerosol layer’s light extinction.</p>

scholarly journals Interactions of meteoric smoke particles with sulphuric acid in the Earth's stratosphere

2012 ◽  
Vol 12 (10) ◽  
pp. 4387-4398 ◽  
Author(s):  
R. W. Saunders ◽  
S. Dhomse ◽  
W. S. Tian ◽  
M. P. Chipperfield ◽  
J. M. C. Plane
Keyword(s):  
Sulphuric Acid ◽  
Climate Model ◽  
Middle Atmosphere ◽  
Magnesium Silicate ◽  
Stratospheric Aerosol ◽  
Solution Viscosity ◽  
Time Resolved ◽  
Optical Extinction ◽  
Smoke Particles ◽  
Meteoric Smoke

Abstract. Nano-sized meteoric smoke particles (MSPs) with iron-magnesium silicate compositions, formed in the upper mesosphere as a result of meteoric ablation, may remove sulphuric acid from the gas-phase above 40 km and may also affect the composition and behaviour of supercooled H2SO4-H2O droplets in the global stratospheric aerosol (Junge) layer. This study describes a time-resolved spectroscopic analysis of the evolution of the ferric (Fe3+) ion originating from amorphous ferrous (Fe2+)-based silicate powders dissolved in varying Wt % sulphuric acid (30–75 %) solutions over a temperature range of 223–295 K. Complete dissolution of the particles was observed under all conditions. The first-order rate coefficient for dissolution decreases at higher Wt % and lower temperature, which is consistent with the increased solution viscosity limiting diffusion of H2SO4 to the particle surfaces. Dissolution under stratospheric conditions should take less than a week, and is much faster than the dissolution of crystalline Fe2+ compounds. The chemistry climate model UMSLIMCAT (based on the UKMO Unified Model) was then used to study the transport of MSPs through the middle atmosphere. A series of model experiments were performed with different uptake coefficients. Setting the concentration of 1.5 nm radius MSPs at 80 km to 3000 cm−3 (based on rocket-borne charged particle measurements), the model matches the reported Wt % Fe values of 0.5–1.0 in Junge layer sulphate particles, and the MSP optical extinction between 40 and 75 km measured by a satellite-borne spectrometer, if the global meteoric input rate is about 20 tonnes per day. The model indicates that an uptake coefficient ≥0.01 is required to account for the observed two orders of magnitude depletion of H2SO4 vapour above 40 km.

scholarly journals Observations of meteoritic material and implications for aerosol nucleation in the winter Arctic lower stratosphere derived from in situ particle measurements

2005 ◽  
Vol 5 (4) ◽  
pp. 5039-5080 ◽  
Author(s):  
J. Curtius ◽  
R. Weigel ◽  
H.-J. Vössing ◽  
H. Wernli ◽  
A. Werner ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Particle Density ◽  
Aerosol Particles ◽  
Potential Temperature ◽  
Polar Vortex ◽  
The Arctic ◽  
Particle Nucleation ◽  
Particle Measurements ◽  
Total Particle

Abstract. Number concentrations of total and non-volatile aerosol particles with size diameters >0.01 µm as well as particle size distributions (0.4–23 µm diameter) were measured in situ in the Arctic lower stratosphere (10–20.5 km altitude). The measurements were obtained during the campaigns European Polar Stratospheric Cloud and Lee Wave Experiment (EUPLEX) and Envisat-Arctic-Validation (EAV). The campaigns were based in Kiruna, Sweden, and took place from January to March 2003. Measurements were conducted onboard the Russian high-altitude research aircraft Geophysica using the low-pressure Condensation Nucleus Counter COPAS (COndensation PArticle Counter System) and a modified FSSP 300 (Forward Scattering Spectrometer Probe). Around 18–20 km altitude typical total particle number concentrations nt range at 10–20 cm−3 (ambient conditions). Correlations with the trace gases nitrous oxide (N2O) and trichlorofluoromethane (CFC-11) are discussed. Inside the polar vortex the total number of particles >0.01 µm increases with potential temperature while N2O is decreasing which indicates a source of particles in the above polar stratosphere or mesosphere. A separate channel of the COPAS instrument measures the fraction of aerosol particles non-volatile at 250°C. Inside the polar vortex a much higher fraction of particles contained non-volatile residues than outside the vortex (~24% outside vortex). This is most likely due to a strongly increased fraction of meteoritic material in the particles which is transported downward from the mesosphere inside the polar vortex. The high fraction of non-volatile residual particles gives therefore experimental evidence for downward transport of mesospheric air inside the polar vortex. It is also shown that the fraction of non-volatile residual particles serves directly as a suitable experimental vortex tracer. Nanometer-sized meteoritic smoke particles may also serve as nuclei for the condensation of gaseous sulfuric acid and water in the polar vortex and these additional particles may be responsible for the increase in the observed particle concentration at low N2O. The number concentrations of particles >0.4 µm measured with the FSSP decrease markedly inside the polar vortex with increasing potential temperature, also a consequence of subsidence of air from higher altitudes inside the vortex. Another focus of the analysis was put on the particle measurements in the lowermost stratosphere. For the total particle density relatively high number concentrations of several hundred particles per cm3 at altitudes below ~14 km were observed in several flights. To investigate the origin of these high number concentrations we conducted air mass trajectory calculations and compared the particle measurements with other trace gas observations. The high number concentrations of total particles in the lowermost stratosphere are probably caused by transport of originally tropospheric air from lower latitudes and are potentially influenced by recent particle nucleation.

scholarly journals Observations of meteoric material and implications for aerosol nucleation in the winter Arctic lower stratosphere derived from in situ particle measurements

2005 ◽  
Vol 5 (11) ◽  
pp. 3053-3069 ◽  
Author(s):  
J. Curtius ◽  
R. Weigel ◽  
H.-J. Vössing ◽  
H. Wernli ◽  
A. Werner ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Aerosol Particles ◽  
Potential Temperature ◽  
Polar Vortex ◽  
The Arctic ◽  
Particle Nucleation ◽  
Particle Measurements ◽  
Total Particle ◽  
Meteoric Material

Abstract. Number concentrations of total and non-volatile aerosol particles with size diameters >0.01 μm as well as particle size distributions (0.4–23 μm diameter) were measured in situ in the Arctic lower stratosphere (10–20.5 km altitude). The measurements were obtained during the campaigns European Polar Stratospheric Cloud and Lee Wave Experiment (EUPLEX) and Envisat-Arctic-Validation (EAV). The campaigns were based in Kiruna, Sweden, and took place from January to March 2003. Measurements were conducted onboard the Russian high-altitude research aircraft Geophysica using the low-pressure Condensation Nucleus Counter COPAS (COndensation PArticle Counter System) and a modified FSSP 300 (Forward Scattering Spectrometer Probe). Around 18–20 km altitude typical total particle number concentrations nt range at 10–20 cm−3 (ambient conditions). Correlations with the trace gases nitrous oxide (N2O) and trichlorofluoromethane (CFC-11) are discussed. Inside the polar vortex the total number of particles >0.01 μm increases with potential temperature while N2O is decreasing which indicates a source of particles in the above polar stratosphere or mesosphere. A separate channel of the COPAS instrument measures the fraction of aerosol particles non-volatile at 250°C. Inside the polar vortex a much higher fraction of particles contained non-volatile residues than outside the vortex (~67% inside vortex, ~24% outside vortex). This is most likely due to a strongly increased fraction of meteoric material in the particles which is transported downward from the mesosphere inside the polar vortex. The high fraction of non-volatile residual particles gives therefore experimental evidence for downward transport of mesospheric air inside the polar vortex. It is also shown that the fraction of non-volatile residual particles serves directly as a suitable experimental vortex tracer. Nanometer-sized meteoric smoke particles may also serve as nuclei for the condensation of gaseous sulfuric acid and water in the polar vortex and these additional particles may be responsible for the increase in the observed particle concentration at low N2O. The number concentrations of particles >0.4 μm measured with the FSSP decrease markedly inside the polar vortex with increasing potential temperature, also a consequence of subsidence of air from higher altitudes inside the vortex. Another focus of the analysis was put on the particle measurements in the lowermost stratosphere. For the total particle density relatively high number concentrations of several hundred particles per cm3 at altitudes below ~14 km were observed in several flights. To investigate the origin of these high number concentrations we conducted air mass trajectory calculations and compared the particle measurements with other trace gas observations. The high number concentrations of total particles in the lowermost stratosphere are probably caused by transport of originally tropospheric air from lower latitudes and are potentially influenced by recent particle nucleation.

scholarly journals Effects of SO<sub>2</sub> oxidation on ambient aerosol growth in water and ethanol vapours

2005 ◽  
Vol 5 (3) ◽  
pp. 767-779 ◽  
Author(s):  
T. Petäjä ◽  
V.-M. Kerminen ◽  
K. Hämeri ◽  
P. Vaattovaara ◽  
J. Joutsensaari ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Sulphuric Acid ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
The Arctic ◽  
Ambient Conditions ◽  
Similar Chemical ◽  
Ethanol Vapours ◽  
Hygroscopic Particles ◽  
Ultrafine Aerosol

Abstract. Hygroscopicity (i.e. water vapour affinity) of atmospheric aerosol particles is one of the key factors in defining their impacts on climate. Condensation of sulphuric acid onto less hygroscopic particles is expected to increase their hygrocopicity and hence their cloud condensation nuclei formation potential. In this study, differences in the hygroscopic and ethanol uptake properties of ultrafine aerosol particles in the Arctic air masses with a different exposure to anthropogenic sulfur pollution were examined. The main discovery was that Aitken mode particles having been exposed to polluted air were more hygroscopic and less soluble to ethanol than after transport in clean air. This aging process was attributed to sulphur dioxide oxidation and subsequent condensation during the transport of these particle to our measurement site. The hygroscopicity of nucleation mode aerosol particles, on the other hand, was approximately the same in all the cases, being indicative of a relatively similar chemical composition despite the differences in air mass transport routes. These particles had also been produced closer to the observation site typically 3–8 h prior to sampling. Apparently, these particles did not have an opportunity to accumulate sulphuric acid on their way to the site, but instead their chemical composition (hygroscopicity and ethanol solubility) resembled that of particles produced in the local or semi-regional ambient conditions.

scholarly journals Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

2016 ◽  
Author(s):  
Martin Ebert ◽  
Ralf Weigel ◽  
Konrad Kandler ◽  
Gebhard Günther ◽  
Sergej Molleker ◽  
...  
Keyword(s):  
Aerosol Particles ◽  
Stratospheric Aerosol ◽  
The Arctic ◽  
Late Winter ◽  
General Tendency ◽  
Polar Stratospheric Clouds ◽  
Metal Mixtures ◽  
Air Masses ◽  
Size And Morphology ◽  
Stratospheric Clouds

Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board of the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed in a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSC). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate-, Fe-rich-, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe early winter, during the late winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate/carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm additionally the presence of soot was proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of such large refractory particles in the stratosphere, and the fact that these particles were not observed in the particle samples (upper size limit about 5 µm) taken during PSC events, strengthen the hypothesis that such particles are present in the polar stratosphere in late winter and that they can provide a surface for heterogeneous condensation during PSC formation.

scholarly journals Technical Note: A novel rocket-based in situ collection technique for mesospheric and stratospheric aerosol particles

2013 ◽  
Vol 6 (3) ◽  
pp. 777-785 ◽  
Author(s):  
W. Reid ◽  
P. Achtert ◽  
N. Ivchenko ◽  
P. Magnusson ◽  
T. Kuremyr ◽  
...  
Keyword(s):  
Electron Microscopy ◽  
Particle Number ◽  
Aerosol Particles ◽  
Stratospheric Aerosol ◽  
Technical Note ◽  
Sounding Rocket ◽  
Height Range ◽  
Transmission Electron ◽  
In Situ Collection

Abstract. A technique for collecting aerosol particles between altitudes of 17 and 85 km is described. Spin-stabilized collection probes are ejected from a sounding rocket allowing for multi-point measurements. Each probe is equipped with 110 collection samples that are 3 mm in diameter. The collection samples are one of three types: standard transmission electron microscopy carbon grids, glass fibre filter paper or silicone gel. Collection samples are exposed over a 50 m to 5 km height range with a total of 45 separate ranges. Post-flight electron microscopy will give size-resolved information on particle number, shape and elemental composition. Each collection probe is equipped with a suite of sensors to capture the probe's status during the fall. Parachute recovery systems along with GPS-based localization will ensure that each probe can be located and recovered for post-flight analysis.

scholarly journals Evidence for long-lived polar vortex air in the mid-latitude summer stratosphere from in situ laser diode CH<sub>4</sub> and H<sub>2</sub>O measurements

2005 ◽  
Vol 5 (6) ◽  
pp. 1467-1472 ◽  
Author(s):  
G. Durry ◽  
A. Hauchecorne
Keyword(s):  
High Resolution ◽  
Laser Diode ◽  
Polar Vortex ◽  
The Arctic ◽  
Concentration Profiles ◽  
Spatial Structures ◽  
Laser Spectrometer ◽  
Southern France ◽  
Diode Laser Spectrometer

Abstract. A balloon borne diode laser spectrometer was launched in southern France in June 2000 to yield in situ stratospheric CH4 and H2O measurements. In the altitude region ranging from 20km to 25km, striking large spatial structures were observed in the vertical concentration profiles of both species. We suggest these patterns are due to the presence of long-lived remnants of the wintertime polar vortex in the mid-latitude summer stratosphere. To support this interpretation, a high resolution advection model for potential vorticity is used to investigate the evolution of the Arctic vortex after its breakdown phase in spring 2000.

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