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

Saunders, R. W.; Dhomse, Sandip; Tian, Wenshou; Chipperfield, Martyn P.; Plane, J. M. C.

doi:10.5194/acp-12-4387-2012

Cited by 53 publications

(63 citation statements)

References 55 publications

(83 reference statements)

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“…The overpredicted nucleation rate in these volcanically quiescent conditions may be a result of gas phase concentrations of H 2 SO 4 being too high in the model. Possible explanations might be that the model does not include the sink for gas phase H 2 SO 4 provided by meteoric debris, shown to be important by Saunders et al (2012) and Brühl et al (2013) or underestimated H 2 SO 4 photolysis rates in our simulations.…”

Section: Particle Size Distributionmentioning

confidence: 95%

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

et al. 2014

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Abstract. We use a stratosphere-troposphere compositionclimate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO 2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H 2 SO 4 . In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO 2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO 2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO 2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations.We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloonborne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41 • N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, Published by Copernicus Publications on behalf of the European Geosciences Union. S. S. Dhomse et al.: Simulation of Pinatubo aerosol in a CCMwhereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescen...

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Section: Particle Size Distributionmentioning

confidence: 95%

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

et al. 2014

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“…Bluhm et al (2010) demonstrated that phytoplankton can reduce IO − 3 to I − , while UV light can also drive the reduction of IO − 3 to I − in seawater (Saunders et al, 2012b;Wong, 1991). Doubts remain regarding iodine inorganic speciation in aerosols and which factors are able to control this speciation ; UV light and ozone have been proposed to play important roles (Saunders et al, 2012a).…”

Section: Introductionmentioning

confidence: 99%

Halogen species record Antarctic sea ice extent over glacial–interglacial periods

Spolaor

Vallelonga²,

Plane

et al. 2013

Atmos. Chem. Phys.

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Sea ice is an integral part of the earth's climate system because it affects planetary albedo, sea-surface salinity, and the atmosphere–ocean exchange of reactive gases and aerosols. Bromine and iodine chemistry is active at polar sea ice margins with the occurrence of bromine explosions and the biological production of organoiodine from sea ice algae. Satellite measurements demonstrate that concentrations of bromine oxide (BrO) and iodine oxide (IO) decrease over sea ice toward the Antarctic interior. Here we present speciation measurements of bromine and iodine in the TALDICE (TALos Dome Ice CorE) ice core (159°11' E, 72°49' S; 2315 m a.s.l.) spanning the last 215 ky. The Talos Dome ice core is located 250 km inland and is sensitive to marine air masses intruding onto the Antarctic Plateau. Talos Dome bromide (Br⁻) is positively correlated with temperature and negatively correlated with sodium (Na). Based on the Br⁻/Na seawater ratio, bromide is depleted in the ice during glacial periods and enriched during interglacial periods. Total iodine, consisting of iodide (I⁻) and iodate (IO₃⁻), peaks during glacials with lower values during interglacial periods. Although IO₃⁻ is considered the most stable iodine species in the atmosphere it was only observed in the TALDICE record during glacial maxima. Sea ice dynamics are arguably the primary driver of halogen fluxes over glacial–interglacial timescales, by altering the distance between the sea ice edge and the Antarctic plateau and by altering the surface area of sea ice available to algal colonization. Based on our results we propose the use of both halogens for examining Antarctic variability of past sea ice extent

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“…These particles are present in sufficient quantities (∼1000's per cm 3 [4]) to play a significant role in a number of atmospheric processes, including cloud nucleation and removal of H 2 SO 4 from the gas phase at high altitude. Laboratory dissolution studies using analogue ANPs provide the physical constraints necessary to assess their environmental impact via modelling [7]. Similarly in astrophysics, Mg-rich pyroxene ANPs condense as dust particles (along with other solid species) in the circumstellar regions surrounding evolved stars and are ubiquitous throughout space.…”

Section: Introductionmentioning

confidence: 99%

Amorphous silicate nanoparticles with controlled Fe-Mg pyroxene compositions

Thompson

Demyk

Day

et al. 2016

Journal of Non-Crystalline Solids

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The production of amorphous pyroxene nanoparticles (∼20 nm) with controlled Fe-Mg content is described. Homogenous particle compositions closely matching required target stoichiometries are obtained by drying a precursor gel under high vacuum conditions. The silicate nature of the particles is characterised using TEM, synchrotron radiation and FTIR. No oxide phase separation occurs, even at high Fe concentration. Structural domains exist within the nanoparticles that are typically ten times smaller than the physical particle size consistent with either a core-shell, or random network with multiple embedded domains, particle structure. Thermal annealing below the crystallisation temperature allows the ordered domain size to be further * Corresponding author reduced by a factor of ∼2.

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

Cited by 53 publications

References 55 publications

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

Halogen species record Antarctic sea ice extent over glacial–interglacial periods

Amorphous silicate nanoparticles with controlled Fe-Mg pyroxene compositions

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