Abstract
SO2 and H2S are the two most important gas-phase sulfur species emitted by volcanoes, with a global amount from non-explosive emissions of the order 10 Tg-S/yr. These gases are readily oxidized forming SO42− aerosols, which effectively scatter the incoming solar radiation and cool the surface. They also perturb atmospheric chemistry by enhancing the NOx to HNO3 heterogeneous conversion via hydrolysis on the aerosol surface of N2O5 and Br-Cl nitrates. This reduces formation of tropospheric O3 and the OH to HO2 ratio, thus limiting the oxidation of CH4 and increasing its lifetime. In addition to this tropospheric chemistry perturbation, there is also an impact on the NOx heterogeneous chemistry in the lower stratosphere, due to vertical transport of volcanic SO2 up to the tropical tropopause layer. Furthermore, the stratospheric O3 formation and loss, as well as the NOx budget, may be slightly affected by the additional amount of upward diffused solar radiation and consequent increase of photolysis rates. Two multi-decadal time-slice runs of a climate-chemistry-aerosol model have been designed for studying these chemical-radiative effects. A tropopause mean global net radiative flux change (RF) of −0.23 W·m−2 is calculated (including direct and indirect aerosol effects) with a 14% increase of the global mean sulfate aerosol optical depth. A 5–15 ppt NOx decrease is found in the mid-troposphere subtropics and mid-latitudes and also from pole to pole in the lower stratosphere. The tropospheric NOx perturbation triggers a column O3 decrease of 0.5–1.5 DU and a 1.1% increase of the CH4 lifetime. The surface cooling induced by solar radiation scattering by the volcanic aerosols induces a tropospheric stabilization with reduced updraft velocities that produce ice supersaturation conditions in the upper troposphere. A global mean 0.9% decrease of the cirrus ice optical depth is calculated with an indirect RF of −0.08 W·m−2.
Highlights
Mineral dust and gas-phase sulfur species are the most important volcanic emissions for aerosols.Primary dust from continuous eruptive activity, represents on average only 1% or less than soil dust emission [1]
The surface cooling induced by solar radiation scattering by the volcanic aerosols induces a tropospheric stabilization with reduced updraft velocities that produce ice supersaturation conditions in the upper troposphere
Except for some overestimation at the northern mid-latitudes in the upper tropospheric and lower stratospheric (UTLS), the ULAQ model is consistent with observations and normally in their uncertainty range
Summary
Mineral dust and gas-phase sulfur species are the most important volcanic emissions for aerosols. Gas phase sulfuric acid would condense onto smaller particles, due to the initial very efficient loss of coarse mode ash particles via gravitational settling In this way, the stratospheric lifetime of volcanic aerosols is prolonged. A more recent study by Kärcher and Lohmann [22] shows that the UT formation of ice crystals is dominated by homogeneous freezing of solution droplets below temperatures of approximately 233 K This physical mechanism is primarily driven by UT temperatures and vertical velocities of adiabatically rising air parcels with higher water vapor content; the aerosol size distribution plays only a minor role. We have used a climate-chemistry-aerosol coupled model to study direct and indirect radiative-chemical perturbations produced by sulfate aerosols from non-explosive volcanic emissions, both in the troposphere and lower stratosphere. An evaluation of model results that are relevant for these processes has been attempted using satellite or aircraft campaign data for aerosol products, UT ice, tropospheric NOx , upper tropospheric and lower stratospheric (UTLS) O3 and ozone column
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