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

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. <br><br> 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. <br><br> The chemistry climate model UMSLIMCAT (based on the UKMO <I>Unified Model</i>) 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.