Saturn's atmospheric response to the large influx of ring material inferred from Cassini INMS measurements

During the Grand Finale stage of the Cassini mission, organic-rich ring material was discovered to be flowing into Saturn's equatorial upper atmosphere at a surprisingly large rate. Through a series of photochemical models, we have examined the consequences of this ring material on the chemistry of Saturn's neutral and ionized atmosphere. We find that if a substantial fraction of this material enters the atmosphere as vapor or becomes vaporized as the solid ring particles ablate upon atmospheric entry, then the ring-derived vapor would strongly affect the composition of Saturn's ionosphere and neutral stratosphere. Our surveys of Cassini infrared and ultraviolet remote-sensing data from the final few years of the mission, however, reveal none of these predicted chemical consequences. We therefore conclude that either (1) the inferred ring influx represents an anomalous, transient situation that was triggered by some recent dynamical event in the ring system that occurred a few months to a few tens of years before the 2017 end of the Cassini mission, or (2) a large fraction of the incoming material must have been entering the atmosphere as small dust particles less than ~100 nm in radius, rather than as vapor or as large particles that are likely to ablate. Future observations or upper limits for stratospheric neutral species such as HC$_3$N, HCN, and CO$_2$ at infrared wavelengths could shed light on the origin, timing, magnitude, and nature of a possible vapor-rich ring-inflow event.Comment: accepted in Icaru

Halogen Chemistry in Volcanic Plumes (Invited)

International audienceVolcanoes release vast amounts of gases and particles in the atmosphere. Volcanic halogens (HF, HCl, HBr, HI) are co-emitted alongside SO2, and observations show rapid formation of BrO and OClO in the plume as it disperses into the troposphere. The development of 1D and Box models (e.g. PlumeChem) that simulate volcanic plume halogen chemistry aims to characterise how volcanic reactive halogens form and quantify their atmospheric impacts. Following recent advances, these models can broadly reproduce the observed downwind BrO/SO2 ratios using "bromine-explosion" chemistry schemes, provided they use a "high-temperature initialisation" to inject radicals (OH, Cl, Br and possibly NOx) which "kick-start" the low-temperature chemistry cycles that convert HBr into reactive bromine (initially as Br2). The modelled rise in BrO/SO2 and subsequent plateau/decline as the plume disperses downwind reflects cycling between reactive bromine, particularly Br-BrO, and BrO-HOBr-BrONO2. BrCl is produced when aerosol becomes HBr-depleted. Recent model simulations suggest this mechanism for reactive chlorine formation can broadly account for OClO/SO2 reported at Mt Etna. Predicted impacts of volcanic reactive halogen chemistry include the formation of HNO3 from NOx and depletion of ozone. This concurs with HNO3 widely reported in volcanic plumes (although the source of NOx remains under question), as well as observations of ozone depletion reported in plumes from several volcanoes (Mt Redoubt, Mt Etna, Eyjafjallajokull). The plume chemistry can transform mercury into more easily deposited and potentially toxic forms, for which observations are limited. Recent incorporation of volcanic halogen chemistry in a 3D regional model of degassing from Ambrym (Vanuatu) also predicts how halogen chemistry causes depletion of OH to lengthen the SO2 lifetime, and highlights the potential for halogen transport from the troposphere to the stratosphere. However, the model parameter-space is vast and only partially constrained by available observations. Reactions on aerosol are a key driver of the chemistry and are affected by uncertainties in both the HOBr reactive uptake coefficient and the aerosol surface area. Recent work has explored the reactive uptake of HOBr on sulfate-rich aerosol, whilst field-measurements at Mt Etna have aimed to quantify the size-resolved primary aerosol emission, towards improving model representations of this highly non-linear volcanic plume halogen chemistry

Halogen Chemistry in Volcanic Plumes (Invited)

International audienceVolcanoes release vast amounts of gases and particles in the atmosphere. Volcanic halogens (HF, HCl, HBr, HI) are co-emitted alongside SO2, and observations show rapid formation of BrO and OClO in the plume as it disperses into the troposphere. The development of 1D and Box models (e.g. PlumeChem) that simulate volcanic plume halogen chemistry aims to characterise how volcanic reactive halogens form and quantify their atmospheric impacts. Following recent advances, these models can broadly reproduce the observed downwind BrO/SO2 ratios using "bromine-explosion" chemistry schemes, provided they use a "high-temperature initialisation" to inject radicals (OH, Cl, Br and possibly NOx) which "kick-start" the low-temperature chemistry cycles that convert HBr into reactive bromine (initially as Br2). The modelled rise in BrO/SO2 and subsequent plateau/decline as the plume disperses downwind reflects cycling between reactive bromine, particularly Br-BrO, and BrO-HOBr-BrONO2. BrCl is produced when aerosol becomes HBr-depleted. Recent model simulations suggest this mechanism for reactive chlorine formation can broadly account for OClO/SO2 reported at Mt Etna. Predicted impacts of volcanic reactive halogen chemistry include the formation of HNO3 from NOx and depletion of ozone. This concurs with HNO3 widely reported in volcanic plumes (although the source of NOx remains under question), as well as observations of ozone depletion reported in plumes from several volcanoes (Mt Redoubt, Mt Etna, Eyjafjallajokull). The plume chemistry can transform mercury into more easily deposited and potentially toxic forms, for which observations are limited. Recent incorporation of volcanic halogen chemistry in a 3D regional model of degassing from Ambrym (Vanuatu) also predicts how halogen chemistry causes depletion of OH to lengthen the SO2 lifetime, and highlights the potential for halogen transport from the troposphere to the stratosphere. However, the model parameter-space is vast and only partially constrained by available observations. Reactions on aerosol are a key driver of the chemistry and are affected by uncertainties in both the HOBr reactive uptake coefficient and the aerosol surface area. Recent work has explored the reactive uptake of HOBr on sulfate-rich aerosol, whilst field-measurements at Mt Etna have aimed to quantify the size-resolved primary aerosol emission, towards improving model representations of this highly non-linear volcanic plume halogen chemistry