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New analysis is presented of the 1.1 mm wavelength absorption lines in Venus' atmosphere that suggested the presence of phosphine. We retrieve a sulphur dioxide observation from the JCMT archive that was simultaneous within a few days of the PH3 1-0 spectrum obtained in June 2017, and demonstrate via a radiative transfer calculation that contamination of PH3 by SO2 was ~10 per cent. We also present ALMA 2019 spectra of PH3 1-0 and an SO2 transition acquired simultaneously, and infer that SO2 line-contamination was ~2 percent (for the least-noisy half of the planetary disc). The contamination-subtracted ALMA and JCMT spectra (of 6-8 sigma confidence) are now consistent with similar absorption-depths at the two epochs. The two values span -1.9(+/-0.2) 10-4 of the continuum signal (which was re-estimated for ALMA), albeit for differing planetary areas. This suggests that the abundance attributed to phosphine in Venus' atmosphere was broadly similar in 2017 and 2019., Comment: v3 is an proofread version of the paper that will appear in print in MNRAS

We recover PH3 in the atmosphere of Venus in data taken with ALMA, using three different calibration methods. The whole-planet signal is recovered with 5.4{\sigma} confidence using Venus bandpass self-calibration, and two simpler approaches are shown to yield example 4.5-4.8{\sigma} detections of the equatorial belt. Non-recovery by Villanueva et al. is attributable to (a) including areas of the planet with high spectral-artefacts and (b) retaining all antenna baselines which raises the noise by a factor ~2.5. We release a data-processing script that enables our whole-planet result to be reproduced. The JCMT detection of PH3 remains robust, with the alternative SO2 attribution proposed by Villanueva et al. appearing inconsistent both in line-velocity and with millimetre-wavelength SO2 monitoring. SO2 contamination of the ALMA PH3-line is minimal. Net abundances for PH3, in the gas column above ~55 km, are up to ~20 ppb planet-wide with JCMT, and ~7 ppb with ALMA (but with signal-loss possible on scales approaching planetary size). Derived abundances will differ if PH3 occupies restricted altitudes - molecules in the clouds will contribute significantly less absorption at line-centre than equivalent numbers of mesospheric molecules - but in the latter zone, PH3 lifetime is expected to be short. Given we recover phosphine, we suggest possible solutions (requiring substantial further testing): a small collisional broadening coefficient could give narrow lines from lower altitude, or a high eddy diffusion coefficient could allow molecules to survive longer at higher altitudes. Alternatively, PH3 could be actively produced by an unknown mechanism in the mesosphere, but this would need to be in addition to cloud-level PH3 detected retrospectively by Pioneer-Venus., Comment: Revised and updated re-analysis of the phosphine spectra in Venus' clouds; Submitted to Nature Astronomy "Matters Arising" on Apr/19/2021

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., Comment: Response to: Snellen I. et al. Astron. Astroph., in press, arXiv:2010:09761 (2020); Villanueva G. et al. Nat. Ast. Matters Arising; arXiv:2010.14305 (2020); Thompson M. Mon. Not. Roy. Astron. Soc., in press, arXiv:2010.15118 (2020); Submitted to Nature Astronomy "Matters Arising" on Dec/10/2020

We first respond to two points raised by Villanueva et al. We show the JCMT discovery spectrum of PH3 can not be re-attributed to SO2, as the line width is larger than observed for SO2 features, and the required abundance would be an extreme outlier. The JCMT spectrum is also consistent with our simple model, constant PH3-abundance with altitude, with no discrepancy in line profile (within data limits); reconciliation with a full photochemical model is the subject of future work. Section 2 presents initial results from re-processed ALMA data. Villanueva et al. noted an issue with bandpass calibration. They have worked on a partially re-processed subset of the ALMA data, so we note where their conclusions, and those of Greaves et al., are now superseded. To summarise: we recover PH3 in Venus' atmosphere with ALMA (~5{\sigma} confidence). Localised abundance appears to peak at ~5-10 parts-per-billion (ppb), with suggestions of spatial variation. Advanced data-products suggest a planet-averaged PH3 abundance ~1-4 ppb, lower than from the earlier ALMA processing (which indicated 7+ ppb). The ALMA data are reconcilable with the JCMT detection (~20 ppb) if there is order-of-magnitude temporal variation; more advanced processing of the JCMT data is underway to check methods. Independent PH3 measurements suggest possible altitude dependence (under ~5 ppb at 60+ km, up to ~100 ppb at 50+ km; see Section 2: Conclusions.). Given that both ALMA and JCMT were working at the limit of observatory capabilities, new spectra should be obtained. The ALMA data in-hand are no longer limited by calibration, but spectral ripples still exist, probably due to size and brightness of Venus in relation to the primary beam. Further, spatial ripples are present, potentially reducing significance of real narrow spectral features., Comment: Response to the Matters Arising: "No phosphine in the atmosphere of Venus" by G. Villanueva et al., preprint at arXiv:2010.14305; v2 contains updated values and additional technical details

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.

Models and observations suggest that ice-particle aggregation at and beyond the snowline dominates the earliest stages of planet-formation, which therefore is subject to many laboratory studies. However, the pressure-temperature gradients in proto-planetary disks mean that the ices are constantly processed, undergoing phase changes between different solid phases and the gas phase. Open questions remain as to whether the properties of the icy particles themselves dictate collision outcomes and therefore how effectively collision experiments reproduce conditions in pro- toplanetary environments. Previous experiments often yielded apparently contradictory results on collision outcomes, only agreeing in a temperature dependence setting in above $\approx$ 210 K. By exploiting the unique capabilities of the NIMROD neutron scattering instrument, we characterized the bulk and surface structure of icy particles used in collision experiments, and studied how these structures alter as a function of temperature at a constant pressure of around 30 mbar. Our icy grains, formed under liquid nitrogen, undergo changes in the crystalline ice-phase, sublimation, sintering and surface pre-melting as they are heated from 103 to 247 K. An increase in the thickness of the diffuse surface layer from $\approx$ 10 to $\approx$ 30 {\AA} ($\approx$ 2.5 to 12 bilayers) proves increased molecular mobility at temperatures above $\approx$ 210 K. As none of the other changes tie-in with the temperature trends in collisional outcomes, we conclude that the surface pre-melting phenomenon plays a key role in collision experiments at these temperatures. Consequently, the pressure-temperature environment, may have a larger influence on collision outcomes than previously thought., Comment: 12 pages, 5 figures

Water in outflows from protostars originates either as a result of gas-phase synthesis from atomic oxygen at T > 200 K, or from sputtered ice mantles containing water ice. We aim to quantify the contribution of the two mechanisms that lead to water in outflows, by comparing observations of gas-phase water to methanol (a grain surface product) towards three low-mass protostars in NGC1333. In doing so, we also quantify the amount of methanol destroyed in outflows. To do this, we make use of JCMT and Herschel-HIFI data of H2O, CH3OH and CO emission lines and compare them to RADEX non-LTE excitation simulations. We find up to one order of magnitude decrease in the column density ratio of CH3OH over H2O as the velocity increases in the line wings up to ~15 km/s. An independent decrease in X(CH3OH) with respect to CO of up to one order of magnitude is also found in these objects. We conclude that gas-phase formation of H2O must be active at high velocities (above 10 km/s, relative to the source velocity) to re-form the water destroyed during sputtering. In addition, the transition from sputtered water at low velocities to formed water at high velocities must be gradual. We place an upper limit of two orders of magnitude on the destruction of methanol by sputtering effects., Comment: 12 pages, 10 figures

In the quest to understand the formation of the building blocks of life, amorphous solid water (ASW) is one of the most widely studied molecular systems. Indeed, ASW is ubiquitous in the cold interstellar medium (ISM), where ASW-coated dust grains provide a catalytic surface for solid phase chemistry, and is believed to be present in the Earth's atmosphere at high altitudes. It has been shown that the ice surface adsorbs small molecules such as CO, N$_2$, or CH$_4$, most likely at OH groups dangling from the surface. Our study presents completely new insights concerning the behaviour of ASW upon selective infrared (IR) irradiation of its dangling modes. When irradiated, these surface H$_2$O molecules reorganise, predominantly forming a stabilised monomer-like water mode on the ice surface. We show that we systematically provoke "hole-burning" effects (or net loss of oscillators) at the wavelength of irradiation and reproduce the same absorbed water monomer on the ASW surface. Our study suggests that all dangling modes share one common channel of vibrational relaxation; the ice remains amorphous but with a reduced range of binding sites, and thus an altered catalytic capacity., Comment: 11 pages, 4 figures, 1 table. Accepted for publication in the Journal of Physical Chemistry Letters

To reveal the formation of planetesimals it is of great importance to understand the collision behavior of the dusty and icy aggregates they have formed from. We present an experimental setup to investigate the aggregation properties in low-velocity collisions of dust aggregates, solid ices and icy aggregates under microgravity conditions. Results from ESA's 45th Parabolic Flight Campaign show that most collisions in the velocity range 0.1 m/s < v_c < 0.5m/s are dominated by a rebound behavior of the projectile dust aggregates and only ~ 5% of the translational kinetic energy is conserved after the encounters., Comment: Cite as Hei{\ss}elmann, D., Fraser, H., & Blum, J. 2007, Proc. 58th Int. Astronautical Congress 2007 (Paris: Int. Astronautical Federation), IAC-07-A2.1.02

In this paper we present results of two novel experimental methods to investigate the collisional behavior of individual macroscopic icy bodies. The experiments reported here were conducted in the microgravity environments of parabolic flights and the Bremen drop tower facility. Using a cryogenic parabolic-flight setup, we were able to capture 41 near-central collisions of 1.5-cm-sized ice spheres at relative velocities between 6 and $22 \mathrm{cm s^{-1}}$. The analysis of the image sequences provides a uniform distribution of coefficients of restitution with a mean value of $\overline{\varepsilon} = 0.45$ and values ranging from $\varepsilon = 0.06$ to 0.84. Additionally, we designed a prototype drop tower experiment for collisions within an ensemble of up to one hundred cm-sized projectiles and performed the first experiments with solid glass beads. We were able to statistically analyze the development of the kinetic energy of the entire system, which can be well explained by assuming a granular `fluid' following Haff's law with a constant coefficient of restitution of $\varepsilon = 0.64$. We could also show that the setup is suitable for studying collisions at velocities of $< 5 \mathrm{mm s^{-1}}$ appropriate for collisions between particles in Saturn's dense main rings., Comment: Accepted for publication in the Icarus Special Issue "Cassini at Saturn"

This paper presents Spitzer-IRS spectroscopy of the CO2 15.2 micron bending mode toward a sample of 50 embedded low-mass stars in nearby star-forming clouds, taken mostly from the ``Cores to Disks (c2d)'' Legacy program. The average abundance of solid CO2 relative to water in low-mass protostellar envelopes is 0.32 +/- 0.02, significantly higher than that found in quiescent molecular clouds and in massive star forming regions. It is found that a decomposition of all the observed CO2 bending mode profiles requires a minimum of five unique components. Roughly 2/3 of the CO2 ice is found in a water-rich environment, while most of the remaining 1/3 is found in a CO environment. Ground-based observations of solid CO toward a large subset of the c2d sample are used to further constrain the CO2:CO component and suggest a model in which low-density clouds form the CO2:H2O component and higher density clouds form the CO2:CO ice during and after the freeze-out of gas-phase CO. It is suggested that the subsequent evolution of the CO2 and CO profiles toward low-mass protostars, in particular the appearance of the splitting of the CO2 bending mode due to pure, crystalline CO2, is first caused by distillation of the CO2:CO component through evaporation of CO due to thermal processing to ~20-30 K in the inner regions of infalling envelopes. The formation of pure CO2 via segregation from the H2O rich mantle may contribute to the band splitting at higher levels of thermal processing (>50 K), but is harder to reconcile with the physical structure of protostellar envelopes around low-luminosity objects., Comment: Accepted for ApJ

At the high densities and low temperatures found in star forming regions, all molecules other than H2 should stick on dust grains on timescales shorter than the cloud lifetimes. Yet these clouds are detected in the millimeter lines of gaseous CO. At these temperatures, thermal desorption is negligible and hence a non-thermal desorption mechanism is necessary to maintain molecules in the gas phase. Here, the first laboratory study of the photodesorption of pure CO ice under ultra high vacuum is presented, which gives a desorption rate of 3E-3 CO molecules per UV (7-10.5 eV) photon at 15 K. This rate is factors of 1E2-1E5 larger than previously estimated and is comparable to estimates of other non-thermal desorption rates. The experiments constrains the mechanism to a single photon desorption process of ice surface molecules. The measured efficiency of this process shows that the role of CO photodesorption in preventing total removal of molecules in the gas has been underestimated., Comment: 5 pages, 4 figures, accepted by ApJL

H2O is the most abundant component of astrophysical ices. In most lines of sight it is not possible to fit both the H2O 3 um stretching, the 6 um bending and the 13 um libration band intensities with a single pure H2O spectrum. Recent Spitzer observations have revealed CO2 ice in high abundances and it has been suggested that CO2 mixed into H2O ice can affect relative strengths of the 3 um and 6 um bands. We used laboratory infrared transmission spectroscopy of H2O:CO2 ice mixtures to investigate the effects of CO2 on H2O ice spectral features at 15-135 K. We find that the H2O peak profiles and band strengths are significantly different in H2O:CO2 ice mixtures compared to pure H2O ice. In all H2O:CO2 mixtures, a strong free-OH stretching band appears around 2.73 um, which can be used to put an upper limit on the CO2 concentration in the H2O ice. The H2O bending mode profile also changes drastically with CO2 concentration; the broad pure H2O band gives way to two narrow bands as the CO2 concentration is increased. This makes it crucial to constrain the environment of H2O ice to enable correct assignments of other species contributing to the interstellar 6 um absorption band. The amount of CO2 present in the H2O ice of B5:IRS1 is estimated by simultaneously comparing the H2O stretching and bending regions and the CO2 bending mode to laboratory spectra of H2O, CO2, H2O:CO2 and HCOOH., Comment: 12 pages, 11 figures, accepted by A&A

A solid-state feature was detected at around 2175 cm-1 towards 30 embedded young stellar objects in spectra obtained using the ESO VLT-ISAAC. We present results from laboratory studies of CO adsorbed at the surface of Zeolite wafers, where absorption bands were detected at 2177 and 2168 cm-1 (corresponding to CO chemisorbed at the Zeolite surface), and 2130 cm-1 (corresponding to CO physisorbed at the Zeolite surface), providing an excellent match to the observational data. We propose that the main carrier of the 2175-band is CO chemisorbed at bare surfaces of dust grains in the interstellar medium. This result provides the first direct evidence that gas-surface interactions do not have to result in the formation of ice mantles on interstellar dust. The strength of the 2175-band is estimated to be ~ 4 x 10-19 cm molecule-1. The abundance of CO adsorbed at bare grain surfaces ranges from 0.06 to 0.16 relative to H2O ice, which is, at most, half of the abundance (relative to H2O ice) of CO residing in H2O-dominated ice environments. These findings imply that interstellar grains have a large (catalytically-active) surface area, providing a refuge for interstellar species. Consequently the potential exists for heterogeneous chemistry to occur involving CO molecules in unique surface chemistry pathways not currently considered in gas-grain models of the interstellar medium., Comment: 19 pages inc. 3 figures 2 tables, accepted for publication in MNRAS

Water (H2O) ice is an important solid constituent of many astrophysical environments. To comprehend the role of such ices in the chemistry and evolution of dense molecular clouds and comets, it is necessary to understand the freeze-out, potential surface reactivity, and desorption mechanisms of such molecular systems. Consequently, there is a real need from within the astronomical modelling community for accurate empirical molecular data pertaining to these processes. Here we give the first results of a laboratory programme to provide such data. Measurements of the thermal desorption of H2O ice, under interstellar conditions, are presented. For ice deposited under conditions that realistically mimic those in a dense molecular cloud, the thermal desorption of thin films (~50 molecular layers) is found to occur with zero order kinetics characterised by a surface binding energy, E_{des}, of 5773 +/- 60 K, and a pre-exponential factor, A, of 10^(30 +/- 2) molecules cm^-2 s^-1. These results imply that, in the dense interstellar medium, thermal desorption of H2O ice will occur at significantly higher temperatures than has previously been assumed., Comment: 9 pages, 4 figures, accepted for publication in MNRAS