Sub-grid scale representation of halogen chemistry in volcanic plumes based on 1D MOCAGE model simulations

Halogen halides emitted by volcanoes are known to rapidly convert within plumes into BrO while depleting ozone, as clearly shown by observations and models over the past 2 decades (e.g. review by Gutmann et al., 2018). So far, most of the modelling studies have focused on the plume processes occurring in the first few hours after the emission. The only study at the regional scale is that of Jourdain et al. (2016). They assessed the impact of volcanic halogens for a period of strong degassing of the Ambrym volcano, showing in particular its effect on the atmospheric oxidizing capacity and methane lifetime.

A step further would be to quantify the impact of volcanic halogens at the global scale using global chemistry models. This type of model uses a horizontal resolution (greater than 50 km) that is much coarser than the plume size. This raises the issue of, whether at this resolution, it is possible to represent the chemistry occurring under high concentrations within the plume. To assess this, a sub-grid scale parameterization is proposed. It has been tested in the 1D version of MOCAGE global and regional chemistry transport model for a short eruption of Mt Etna on the 10^th of May 2008. The results show that while using the subgrid-scale plume parameterization or not does change the timing of when the maximum BrO occurs but does not affect the predicted maximum concentration. The same finding is made when using a range of different settings in the parameterization regarding dilution of the plume with its environment. The 1D model results show a sensitivity of BrO formation to parameters other than the sub-grid scale effects: composition of the plume at the vent, injection height of the emissions, and time of the day when the eruption takes place.