Abstract

We investigated the role of the passive volcanic plume of Mount Etna (Italy) in the formation of new particles in the size range of 2.5–10 nm through the gas-to-particle nucleation of sulfuric acid (H2SO4) precursors, formed from the oxidation of SO2, and their evolution to particles with diameters larger than 100 nm. Two simulations were performed using the Weather Research and Forecasting Model coupled with chemistry (WRF-Chem) under the same configuration, except for the nucleation parameterization implemented in the model: the activation nucleation parameterization (JS1 = 2.0 × 10−6 × (H2SO4)) in the first simulation (S1) and a new parameterization for nucleation (NPN) (JS2 = 1.844 × 10−8 × (H2SO4)1.12) in the second simulation (S2). The comparison of the numerical results with the observations shows that, on average, NPN improves the performance of the model in the prediction of the H2SO4 concentrations, newly-formed particles (~2.5–10 nm), and their growth into larger particles (10–100 nm) by decreasing the rates of H2SO4 consumption and nucleation relative to S1. In addition, particles formed in the plume do not grow into cloud condensation nuclei (CCN) sizes (100–215 nm) within a few hours of the vent (tens of km). However, tracking the size evolution of simulated particles along the passive plume indicates the downwind formation of particles larger than 100 nm more than 100 km far from the vent with relatively high concentrations relative to the background (more than 1500 cm−3) in S2. These particles, originating in the volcanic source, could affect the chemical and microphysical properties of clouds and exert regional climatic effects over time.

Highlights

  • Volcanic eruption and passive degassing are among the main natural sources of several atmospheric gaseous species and particles, primarily emitted or secondarily newly-formed particles [1]

  • This potential impact on climate arises from the higher efficiency of volcanic sulfur at producing sulfate aerosols, which is thought to be 4.5 times higher than that of anthropogenic sulfur because volcanic SO2 molecules released at high tropospheric altitudes feature a longer residence time; this is mainly due to their appreciably lower dry deposition rate compared to that of anthropogenic SO2 emitted at surface level [5,6]

  • Volcanic passive degassing in the troposphere has long-lasting impacts on the safety of air traffic, air pollution, and local/regional climates through the emission of gases and particles at both local and regional scales [126]

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Summary

Introduction

Volcanic eruption and passive degassing are among the main natural sources of several atmospheric gaseous species and particles, primarily emitted or secondarily newly-formed particles [1]. The anthropogenic SO2 source intensity is about five times greater than volcanic emissions, the radiative effects of volcanic sulfates are only slightly weaker than those induced by anthropogenic sulfates. This potential impact on climate arises from the higher efficiency of volcanic sulfur at producing sulfate aerosols, which is thought to be 4.5 times higher than that of anthropogenic sulfur because volcanic SO2 molecules released at high tropospheric altitudes feature a longer residence time; this is mainly due to their appreciably lower dry deposition rate compared to that of anthropogenic SO2 emitted at surface level [5,6]. An increase in CCN, for clouds of equal liquid water content, enhances the concentration of cloud droplets and reduces their size

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