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Register a new userHydroxide salts in the clouds of Venus: their effect on the sulfur cycle and cloud droplet pH
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The depletion of SO$_2$ and H$_2$O in and above the clouds of Venus (45 -- 65 km) cannot be explained by known gas-phase chemistry and the observed composition of the atmosphere. We apply a full-atmosphere model of Venus to investigate three potential explanations for the SO$_2$ and H$_2$O depletion: (1) varying the below-cloud water vapor (H$_2$O), (2) varying the below-cloud sulfur dioxide (SO$_2$), and (3) the incorporation of chemical reactions inside the sulfuric acid cloud droplets. We find that increasing the below-cloud H$_2$O to explain the SO$_2$ depletion results in a cloud top that is 20 km too high, above-cloud O$_2$ three orders of magnitude greater than observational upper limits and no SO above 80 km. The SO$_2$ depletion can be explained by decreasing the below-cloud SO$_2$ to $20,{rm ppm}$. The depletion of SO$_2$ in the clouds can also be explained by the SO$_2$ dissolving into the clouds, if the droplets contain hydroxide salts. These salts buffer the cloud pH. The amount of salts sufficient to explain the SO$_2$ depletion entail a droplet pH of $sim 1$ at 50 km. Since sulfuric acid is constantly condensing out into the cloud droplets, there must be a continuous and pervasive flux of salts of $approx 10^{-13} , {rm mol , cm^{-2} , s^{-1}}$ driving the cloud droplet chemistry. An atmospheric probe can test both of these explanations by measuring the pH of the cloud droplets and the concentrations of gas-phase SO$_2$ below the clouds.
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Following the announcement of the detection of phosphine (PH$_3$) in the cloud deck of Venus at millimeter wavelengths, we have searched for other possible signatures of this molecule in the infrared range. Since 2012, we have been observing Venus in the thermal infrared at various wavelengths to monitor the behavior of SO$_2$ and H$_2$O at the cloud top. We have identified a spectral interval recorded in March 2015 around 950 cm$^{-1}$ where a PH$_3$ transition is present. From the absence of any feature at this frequency, we derive, on the disk-integrated spectrum, a 3-$sigma$ upper limit of 5 ppbv for the PH$_3$ mixing ratio, assumed to be constant throughout the atmosphere. This limit is 4 times lower than the disk-integrated mixing ratio derived at millimeter wavelengths. Our result brings a strong constraint on the maximum PH$_3$ abundance at the cloud top and in the lower mesosphere of Venus.
The observation of a 266.94 GHz feature in the Venus spectrum has been attributed to PH$_3$ in the Venus clouds, suggesting unexpected geological, chemical or even biological processes. Since both PH$_3$ and SO$_2$ are spectrally active near 266.94 GHz, the contribution to this line from SO$_2$ must be determined before it can be attributed, in whole or part, to PH$_3$. An undetected SO$_2$ reference line, interpreted as an unexpectedly low SO$_2$ abundance, suggested that the 266.94 GHz feature could be attributed primarily to PH$_3$. However, the low SO$_2$ and the inference that PH$_3$ was in the cloud deck posed an apparent contradiction. Here we use a radiative transfer model to analyze the PH$_3$ discovery, and explore the detectability of different vertical distributions of PH$_3$ and SO$_2$. We find that the 266.94 GHz line does not originate in the clouds, but above 80 km in the Venus mesosphere. This level of line formation is inconsistent with chemical modeling that assumes generation of PH$_3$ in the Venus clouds. Given the extremely short chemical lifetime of PH$_3$ in the Venus mesosphere, an implausibly high source flux would be needed to maintain the observed value of 20$pm$10 ppb. We find that typical Venus SO$_2$ vertical distributions and abundances fit the JCMT 266.94 GHz feature, and the resulting SO$_2$ reference line at 267.54 GHz would have remained undetectable in the ALMA data due to line dilution. We conclude that nominal mesospheric SO$_2$ is a more plausible explanation for the JCMT and ALMA data than PH$_3$.
We published spectra of phosphine molecules in Venus clouds, following open-science principles in releasing data and scripts (with community input leading to ALMA re-processing, now benefiting multiple projects). Some misconceptions about de-trending of spectral baselines have also emerged, which we address here. Using the JCMT PH3-discovery data, we show that mathematically-correct polynomial fitting of periodic ripples does not lead to fake lines (probability < ~1%). We then show that the ripples can be characterised in a non-subjective manner via Fourier transforms. A 20 ppb PH3 feature is ~5{sigma} compared to the JCMT baseline-uncertainty, and is distinctive as a narrow perturber of the periodic ripple pattern. The structure of the FT-derived baseline also shows that polynomial fitting, if unguided, can amplify artefacts and so artificially reduce significance of real lines.
Measurements of trace-gases in planetary atmospheres help us explore chemical conditions different to those on Earth. Our nearest neighbor, Venus, has cloud decks that are temperate but hyper-acidic. We report the apparent presence of phosphine (PH3) gas in Venusian atmosphere, where any phosphorus should be in oxidized forms. Single-line millimeter-waveband spectral detections (quality up to ~15 sigma) from the JCMT and ALMA telescopes have no other plausible identification. Atmospheric PH3 at ~20 parts-per-billion abundance is inferred. The presence of phosphine is unexplained after exhaustive study of steady-state chemistry and photochemical pathways, with no currently-known abiotic production routes in Venusian atmosphere, clouds, surface and subsurface, or from lightning, volcanic or meteoritic delivery. Phosphine could originate from unknown photochemistry or geochemistry, or, by analogy with biological production of phosphine on Earth, from the presence of life. Other PH3 spectral features should be sought, while in-situ cloud and surface sampling could examine sources of this gas.
Planetary-scale waves are thought to play a role in powering the yet-unexplained atmospheric superrotation of Venus. Puzzlingly, while Kelvin, Rossby and stationary waves manifest at the upper clouds (65--70 km), no planetary-scale waves or stationary patterns have been reported in the intervening level of the lower clouds (48--55 km), although the latter are probably Lee waves. Using observations by the Akatsuki orbiter and ground-based telescopes, we show that the lower clouds follow a regular cycle punctuated between 30$^{circ}$N--40$^{circ}$S by a sharp discontinuity or disruption with potential implications to Venuss general circulation and thermal structure. This disruption exhibits a westward rotation period of $sim$4.9 days faster than winds at this level ($sim$6-day period), alters clouds properties and aerosols, and remains coherent during weeks. Past observations reveal its recurrent nature since at least 1983, and numerical simulations show that a nonlinear Kelvin wave reproduces many of its properties.
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