Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N

We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (> 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (< 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.

Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68° N

In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68° N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analyzed, of which 147 338 particles were measured in the stratosphere. Of these particles, 50 688 were characterized by high abundances of magnesium, iron, and rare iron oxide compounds, together with sulfuric acid. This particle type was found almost exclusively in the stratosphere (48 610 particles) and is interpreted as meteoric material immersed or dissolved within stratospheric sulfuric acid particles. Below the tropopause, the observed fraction of this particle type decreases sharply. However, small fractional abundances were observed below 3000 m a.s.l. in the Canadian Arctic and also at the Jungfraujoch high altitude station (3600 m a.s.l.). Thus, the removal pathway by sedimentation and/or mixing into the troposphere is confirmed. In the tropical lower stratosphere, only a small fraction (

What controls nucleation of ice and nitric acid hydrates by meteoric material?

&lt;p&gt;Nucleation of crystalline ice and nitric acid hydrates in Polar Stratospheric Clouds (PSC) is important for the destruction of ozone, both through changing the rate of activation of ozone destroying species and through the removal by sedimentation of nitric acid, which can deactivate ozone destroying species. Nucleation is thought to proceed heterogeneously on fragmented meteoric materials, leading to formation of ice and nitric acid trihydrate. The heterogeneous nature of meteoric materials and the potential to form multiple crystalline phases makes this system particularly complex. In particular, the characteristics of meteoric fragments which allow them to nucleate crystallisation in PSCs are unknown. We have investigated the nature of nucleation of nitric acid solutions on meteorite thin section surfaces. We find that nucleation occurs on a range of sites on the surface without significant reproduction in repeat freezing experiments. Electron microscopy showed significant diversity in the type of surface features present in regions where nucleation was observed. This is in contrast to recent studies of ice nucleation on K-feldspar and quartz surfaces, where particular sites were found to dominate nucleation. We also observed a range of different crystalline phases forming competitively, some of which are not represented on the HNO&lt;sub&gt;3&lt;/sub&gt; / H&lt;sub&gt;2&lt;/sub&gt;O equilibrium phase diagram. The results reinforce the complexity of nucleation in PSC and do not support simplifying assumptions commonly made in the literature e.g. around the order in which phases form. In order to facilitate a predictive capacity of future trends in ozone loss significant work is required in understanding the nucleation of nitric acid hydrates by meteoric material.&lt;/p&gt;

Nucleation of nitric acid hydrates in polar stratospheric clouds by meteoric material

Heterogeneous nucleation of crystalline nitric acid hydrates in polar stratospheric clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT, or other nitric acid phases), but this has never been quantitatively demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere: smoke that results from the ablation and re-condensation of vapours, and fragments that result from the break-up of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.

Nucleation of nitric acid hydrates in Polar Stratospheric Clouds by meteoric material

Heterogeneous nucleation of crystalline nitric acid hydrates in Polar Stratospheric Clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT), but this has never been directly demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere, smoke which results from the ablation and re-condensation of vapours, and fragments which result from the disruption of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.