The newly launched imaging spectrometer TROPOMI onboard the Sentinel-5 Precursor satellite provides atmospheric column measurements of sulfur dioxide (SO2) and other gases with a pixel resolution of 3.5 × 7 km2. This permits mapping emission plumes from a vast number of natural and anthropogenic emitters with unprecedented sensitivity, revealing sources which were previously undetectable from space. Novel analysis using back-trajectory modelling of satellite-based SO2 columns allows calculation of SO2 flux time series, which would be of great utility and scientific interest if applied globally. Volcanic SO2 emission time series reflect magma dynamics and are used for risk assessment and calculation of the global volcanic CO2 gas flux. TROPOMI data make this flux time series reconstruction approach possible with unprecedented spatiotemporal resolution, but these new data must be tested and validated against ground-based observations. Mt. Etna (Italy) emits SO2 with fluxes ranging typically between 500 and 5000 t/day, measured automatically by the largest network of scanning UV spectrometers in the world, providing the ideal test-bed for this validation. A comparison of three SO2 flux datasets, TROPOMI (one month), ground-network (one month), and ground-traverse (two days) shows acceptable to excellent agreement for most days. The result demonstrates that reliable, nearly real-time, high temporal resolution SO2 flux time series from TROPOMI measurements are possible for Etna and, by extension, other volcanic and anthropogenic sources globally. This suggests that global automated real-time measurements of large numbers of degassing volcanoes world-wide are now possible, revolutionizing the quantity and quality of magmatic degassing data available and insights into volcanic processes to the volcanological community.

Accurate quantification of the emission rate of sulphur dioxide (SO 2 ) from volcanoes provides both insights into magmatic processes and a powerful monitoring tool for hazard mitigation. The primary method for measuring magmatic SO 2 is Differential Optical Absorption Spectroscopy (DOAS) of UV scattered sunlight spectra, in which a reference spectrum taken outside the plume is used to quantify the SO 2 slant column density inside the plume. This can lead to problems if the reference spectrum is contaminated with SO 2 as this will result in a systematic underestimation of the retrieved SO 2 slant column density, and therefore emission rate. We present a new analysis method, named "iFit", which retrieves the SO 2 slant column density from UV spectra by directly fitting the measured intensity spectrum at high spectral resolution (0.01 nm) using a literature solar reference spectrum and measured instrument characteristics. This eliminates the requirement for a measured reference spectrum, providing a "point and shoot" method for quantifying SO 2 slant column densities. We show that iFit retrieves correct SO 2 slant column densities in a series of test cases, finding agreement with existing methods. We propose that iFit is suitable for both traverse measurements and permanent scanning stations, and could be integrated into volcano monitoring networks at observatories. Finally, we provide an open source software implementation of iFit with a user friendly graphical interface to allow users to easily utilise iFit.

High precision and accuracy in volcanic SO 2 emission rate quantification is critical for eruption forecasting and, in combination with in-plume gas ratios, quantifying global volcanic emission inventories. Light dilution, where scattering of ultraviolet light dilutes plume SO 2 absorbance signals, has been recognized for more than 50 years, but is still not routinely corrected for during gas flux quantification. Here we use modeling and empirical observations from Masaya volcano, Nicaragua, to show that light dilution produces: i) underestimates in SO 2 that can reach a factor of 5 and, at low column densities, cause little impact on standard retrieval fit quality, even for heavily diluted spectra; ii) retrieved SO 2 amounts that are capped by a maximum value regardless of the true amount of SO 2 , with this maximum amount being reduced as light dilution increases. Global volcanic volatile emission rates may therefore be significantly underestimated. An easily implementable dual-waveband analysis provides a means to detect, and in clear sky conditions, correct dilution effects directly from the spectra, opening a path to more accurate SO 2 quantifications.

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Abstract. Knowledge of sulfur dioxide layer height (SO2 LH) is important to understand volcanic eruption processes, the climate impact of SO2 emissions and to mitigate volcanic risk for civil aviation. However, the estimation of SO2 LH from ground-based instruments is challenging in particular for rapidly evolving and sustained eruptions. Satellite wide-swath nadir observations have the advantage to cover large-scale plumes and the potential to provide key information on SO2 LH. In the ultraviolet, SO2 LH retrievals leverage the fact that, for large SO2 columns, the light path and its associated air mass factor (AMF) depends on the SO2 absorption (and therefore on the vertical distribution of SO2), and SO2 LH information can be obtained from the analysis of measured back-scattered radiances coupled with radiative transfer simulations. However, existing algorithms are mainly sensitive to SO2 LH for SO2 vertical columns of at least 20 DU. Here we develop a new SO2 LH algorithm and apply it to observations from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI). It is based on an SO2 optical depth look-up table and an iterative approach. The strength of this scheme lies in the fact that it is a Covariance-Based Retrieval Algorithm (COBRA; Theys et al., 2021). This means that the SO2-free contribution of the measured optical depth is treated in an optimal way, resulting in an improvement of the SO2 LH sensitivity to SO2 columns as low as 5 DU, with a precision better than 2 km. We demonstrate the value of this new data through a number of examples and comparison with satellite plume height estimates (from IASI and CALIOP), and back-trajectory analyses. The comparisons indicate an SO2 LH accuracy of 1–2 km, except for some difficult observation conditions, in particular for optically thick ash plumes or partially SO2-filled scenes.