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Titan's atmospheric composition and dynamical state have previously been studied over numerous epochs by both ground- and space-based facilities. However, stratospheric measurements remain sparse during Titan's northern summer and fall. The lack of seasonal symmetry in observations of Titan's temperature field and chemical abundances raises questions about the nature of the middle atmosphere's meridional circulation and evolution over Titan's 29-yr seasonal cycle that can only be answered through long-term monitoring campaigns. Here, we present maps of Titan's stratospheric temperature, acetonitrile (or methyl cyanide; CH$_3$CN), and monodeuterated methane (CH$_3$D) abundances following Titan's northern summer solstice obtained with Band 9 ($\sim0.43$ mm) ALMA observations. We find that increasing temperatures towards high-southern latitudes, currently in winter, resemble those observed during Titan's northern winter by the Cassini mission. Acetonitrile abundances have changed significantly since previous (sub)millimeter observations, and we find that the species is now highly concentrated at high-southern latitudes. The stratospheric CH$_3$D content is found to range between 4-8 ppm in these observations, and we infer the CH$_4$ abundance to vary between $\sim0.9-1.6\%$ through conversion with previously measured D/H values. A global value of CH$_4=1.15\%$ was retrieved, lending further evidence to the temporal and spatial variability of Titan's stratospheric methane when compared with previous measurements. Additional observations are required to determine the cause and magnitude of stratospheric enhancements in methane during these poorly understood seasons on Titan., Comment: Accepted for publication in the Planetary Science Journal. 9 Figures, 1 table

The study of planets and small bodies within our Solar System is fundamental for understanding the formation and evolution the Earth and other planets. Compositional and meteorological studies of the giant planets provide a foundation for understanding the nature of the most commonly observed exoplanets, while spectroscopic observations of the atmospheres of terrestrial planets, moons, and comets provide insights into the past and present-day habitability of planetary environments, and the availability of the chemical ingredients for life. While prior and existing (sub)millimeter observations have led to major advances in these areas, progress is hindered by limitations in the dynamic range, spatial and temporal coverage, as well as sensitivity of existing telescopes and interferometers. Here, we summarize some of the key planetary science use cases that factor into the design of the Atacama Large Aperture Submillimeter Telescope (AtLAST), a proposed 50-m class single dish facility: (1) to more fully characterize planetary wind fields and atmospheric thermal structures, (2) to measure the compositions of icy moon atmospheres and plumes, (3) to obtain detections of new, astrobiologically relevant gases and perform isotopic surveys of comets, and (4) to perform synergistic, temporally-resolved measurements in support of dedicated interplanetary space missions. The improved spatial coverage (several arcminutes), resolution ($\sim1.2''-12''$), bandwidth (several tens of GHz), dynamic range ($\sim10^5$) and sensitivity ($\sim1$ mK km s$^{-1}$) required by these science cases would enable new insights into the chemistry and physics of planetary environments, the origins of prebiotic molecules and the habitability of planetary systems in general., Comment: Submitted to Open Research Europe (AtLAST collection). 19 pages

Spectral observations of Neptune made in 2019 with the MUSE instrument at the Very Large Telescope in Chile have been analysed to determine the spatial variation of aerosol scattering properties and methane abundance in Neptune's atmosphere. The darkening of the South Polar Wave (SPW) at $\sim$ 60$^\circ$S, and dark spots such as the Voyager 2 Great Dark Spot is concluded to be due to a spectrally-dependent darkening ($\lambda < 650$nm) of particles in a deep aerosol layer at $\sim$ 5 bar and presumed to be composed of a mixture of photochemically-generated haze and H$_2$S ice. We also note a regular latitudinal variation of reflectivity at wavelengths of very low methane absorption longer than $\sim$ 650 nm, with bright zones latitudinally separated by $\sim$ 25$^\circ$. This feature, similar to the spectral characteristics of a discrete deep bright spot DBS-2019 found in our data, is found to be consistent with a brightening of the particles in the same $\sim$5-bar aerosol layer at $\lambda > 650 $ nm. We find the properties of an overlying methane/haze aerosol layer at $\sim$ 2 bar are, to first-order, invariant with latitude, while variations in the opacity of an upper tropospheric haze layer reproduce the observed reflectivity at methane-absorbing wavelengths, with higher abundances found at the equator and also in a narrow `zone' at $80^\circ$S. Finally, we find the mean abundance of methane below its condensation level to be 6--7% at the equator reducing to $\sim$3% south of $\sim$25$^\circ$S, although the absolute abundances are model dependent., Comment: 32 pages, 13 figures. Accepted in JGR: Planets

Previous observations of dark vortices in Neptune's atmosphere, such as Voyager-2's Great Dark Spot, have been made in only a few, broad-wavelength channels, which has hampered efforts to pinpoint their pressure level and what makes them dark. Here, we present Very Large Telescope (Chile) MUSE spectrometer observations of Hubble Space Telescope's NDS-2018 dark spot, made in 2019. These medium-resolution 475 - 933 nm reflection spectra allow us to show that dark spots are caused by a darkening at short wavelengths (< 700 nm) of a deep ~5-bar aerosol layer, which we suggest is the H$_2$S condensation layer. A deep bright spot, named DBS-2019, is also visible on the edge of NDS-2018, whose spectral signature is consistent with a brightening of the same 5-bar layer at longer wavelengths (> 700 nm). This bright feature is much deeper than previously studied dark spot companion clouds and may be connected with the circulation that generates and sustains such spots., Comment: 1 table. 3 figures. Nature Astronomy (2023)

We present a reanalysis (using the Minnaert limb-darkening approximation) of visible/near-infrared (0.3 - 2.5 micron) observations of Uranus and Neptune made by several instruments. We find a common model of the vertical aerosol distribution that is consistent with the observed reflectivity spectra of both planets, consisting of: 1) a deep aerosol layer with a base pressure > 5-7 bar, assumed to be composed of a mixture of H2S ice and photochemical haze; 2) a layer of photochemical haze/ice, coincident with a layer of high static stability at the methane condensation level at 1-2 bar; and 3) an extended layer of photochemical haze, likely mostly of the same composition as the 1-2-bar layer, extending from this level up through to the stratosphere, where the photochemical haze particles are thought to be produced. For Neptune, we find that we also need to add a thin layer of micron-sized methane ice particles at ~0.2 bar to explain the enhanced reflection at longer methane-absorbing wavelengths. We suggest that methane condensing onto the haze particles at the base of the 1-2-bar aerosol layer forms ice/haze particles that grow very quickly to large size and immediately 'snow out' (as predicted by Carlson et al. 1988), re-evaporating at deeper levels to release their core haze particles to act as condensation nuclei for H2S ice formation. In addition, we find that the spectral characteristics of 'dark spots', such as the Voyager-2/ISS Great Dark Spot and the HST/WFC3 NDS-2018, are well modelled by a darkening or possibly clearing of the deep aerosol layer only., Comment: 58 pages, 23 figures, 4 tables

In response to ESA Voyage 2050 announcement of opportunity, we propose an ambitious L-class mission to explore one of the most exciting bodies in the Solar System, Saturn largest moon Titan. Titan, a "world with two oceans", is an organic-rich body with interior-surface-atmosphere interactions that are comparable in complexity to the Earth. Titan is also one of the few places in the Solar System with habitability potential. Titan remarkable nature was only partly revealed by the Cassini-Huygens mission and still holds mysteries requiring a complete exploration using a variety of vehicles and instruments. The proposed mission concept POSEIDON (Titan POlar Scout/orbitEr and In situ lake lander DrONe explorer) would perform joint orbital and in situ investigations of Titan. It is designed to build on and exceed the scope and scientific/technological accomplishments of Cassini-Huygens, exploring Titan in ways that were not previously possible, in particular through full close-up and in situ coverage over long periods of time. In the proposed mission architecture, POSEIDON consists of two major elements: a spacecraft with a large set of instruments that would orbit Titan, preferably in a low-eccentricity polar orbit, and a suite of in situ investigation components, i.e. a lake lander, a "heavy" drone (possibly amphibious) and/or a fleet of mini-drones, dedicated to the exploration of the polar regions. The ideal arrival time at Titan would be slightly before the next northern Spring equinox (2039), as equinoxes are the most active periods to monitor still largely unknown atmospheric and surface seasonal changes. The exploration of Titan northern latitudes with an orbiter and in situ element(s) would be highly complementary with the upcoming NASA New Frontiers Dragonfly mission that will provide in situ exploration of Titan equatorial regions in the mid-2030s., Comment: arXiv admin note: substantial text overlap with arXiv:1908.01374

Herschel/SPIRE observations of Uranus are used to search for stratospheric hydrogen chloride (HCl) emission at 41.74 cm$^{-1}$. HCl was not detected and instead 3$\sigma$ upper limits were determined; $<$6.2 ppb ($<$2.0$\times$10$^{14}$ molecules/cm$^{2}$) for a 0.1 mbar step profile and $<$0.40 ppb ($<$1.2$\times$10$^{14}$ molecules/cm$^{2}$) for a 1 mbar step profile. HCl is expected to have an external source and these upper limits are consistent with abundances of other external species (CO, H$_2$O, CO$_2$) and a solar composition source., Comment: 4 pages, 1 figure, accepted for publication in RNAAS 2020

We report the first detection on Titan of the small cyclic molecule cyclopropenylidene (c-C3H2) from high sensitivity spectroscopic observations made with the Atacama Large Millimeter/sub-millimeter Array (ALMA). Multiple lines of cyclopropenylidene were detected in two separate datasets: ~251 GHz in 2016 (Band 6) and ~352 GHz in 2017 (Band 7). Modeling of these emissions indicates abundances of 0.50 +/- 0.14 ppb (2016) and 0.28 +/- 0.08 (2017) for a 350 km step model, which may either signify a decrease in abundance, or a mean value of 0.33 +/- 0.07 ppb. Inferred column abundances are (3-5)E12 cm-2 in 2016 and (1-2)E12 cm-2 in 2017, similar to photochemical model predictions. Previously the C3H3+ ion has been measured in Titan's ionosphere by Cassini's Ion and Neutral Mass Spectrometer (INMS), but the neutral (unprotonated) species has not been detected until now, and aromatic versus aliphatic structure could not be determined by the INMS. Our work therefore represents the first unambiguous detection of cyclopropenylidene, the second known cyclic molecule in Titan's atmosphere along with benzene (C6H6) and the first time this molecule has been detected in a planetary atmosphere. We also searched for the N-heterocycle molecules pyridine and pyrimidine finding non-detections in both cases, and determining 2-{\sigma} upper limits of 1.15 ppb (c-C5H5N) and 0.85 ppb (c-C4H4N2) for uniform abundances above 300 km. These new results on cyclic molecules provide fresh constraints on photochemical pathways in Titan's atmosphere, and will require new modeling and experimental work to fully understand the implications for complex molecule formation., Comment: 34 pages, 13 figures. 8 tables

We outline a flagship-class mission concept focused on studying Titan as a global system, with particular emphasis on the polar regions. Investigating Titan from the unique standpoint of a polar orbit would enable comprehensive global maps to uncover the physics and chemistry of the atmosphere, and the topography and geophysical environment of the surface and subsurface. The mission includes two key elements: (1) an orbiter spacecraft, which also acts as a data relay, and (2) one or more small probes to directly investigate Titan's seas and make the first direct measurements of their liquid composition and physical environment. The orbiter would carry a sophisticated remote sensing payload, including a novel topographic lidar, a long-wavelength surface-penetrating radar, a sub-millimeter sounder for winds and for mesospheric/thermospheric composition, and a camera and near-infrared spectrometer. An instrument suite to analyze particles and fields would include a mass spectrometer to focus on the interactions between Titan's escaping upper atmosphere and the solar wind and Saturnian magnetosphere. The orbiter would enter a stable polar orbit around 1500 to 1800 km, from which vantage point it would make global maps of the atmosphere and surface. One or more probes, released from the orbiter, would investigate Titan's seas in situ, including possible differences in composition between higher and lower latitude seas, as well as the atmosphere during the parachute descent. The number of probes, as well as the instrument complement on the orbiter and probe, remain to be finalized during a mission study that we recommend to NASA as part of the NRC Decadal Survey for Planetary Science now underway, with the goal of an overall mission cost in the "small flagship" category of ~$2 bn. International partnerships, similar to Cassini-Huygens, may also be included for consideration., Comment: 13 pages, white paper submitted to the NRC Decadal Survey for Planetary Science and Astrobiology

The atmosphere of Titan, the largest moon of Saturn, is rich in organic molecules, and it has been suggested that the moon may serve as an analog for the pre-biotic Earth due to its highly reducing chemistry and existence of global hazes. Photochemical models of Titan have predicted the presence of propadiene (historically referred to as allene), CH$_{2}$CCH$_{2}$, an isomer of the well-measured propyne (also called methylacetylene) CH$_{3}$CCH, but its detection has remained elusive due to insufficient spectroscopic knowledge of the molecule - which has recently been remedied with an updated spectral line list. Here we present the first unambiguous detection of the molecule in any astronomical object, observed with the Texas Echelle Cross Echelle Spectrograph (TEXES) on the NASA Infrared Telescope Facility (IRTF) in July 2017. We model its emission line near 12 $\mu$m and measure a volume mixing ratio (VMR) of (6.9 $\pm$ 0.8) $\times$10$^{-10}$ at 175 km, assuming a vertically increasing abundance profile as predicted in photochemical models. Cassini measurements of propyne made during April 2017 indicate that the abundance ratio of propyne to propadiene is 8.2$\pm$1.1 at the same altitude. This initial measurement of the molecule in Titan's stratosphere paves the way towards constraining the amount of atomic hydrogen available on Titan, as well as future mapping of propadiene on Titan from 8 meter and larger ground based observatories, and future detection on other planetary bodies.

The Cassini Composite Infrared Spectrometer (CIRS) observed thermal emission in the far- and mid-infrared (from 10 cm$^{-1}$ to 1500 cm$^{-1}$), enabling spatiotemporal studies of ethane on Titan across the span of the Cassini mission from 2004 through 2017. Many previous measurements of ethane on Titan have relied on modeling the molecule's mid-infrared $\nu_{12}$ band, centered on 822 cm$^{-1}$. Other bands of ethane at shorter and longer wavelengths were seen, but have not been modeled to measure ethane abundance. Spectral line lists of the far-infrared $\nu_{4}$ torsional band at 289 cm$^{-1}$ and the mid-infrared $\nu_{8}$ band centered ay 1468 cm$^{-1}$ have recently been studied in the laboratory. We model CIRS observations of each of these bands (along with the $\nu_{12}$ band) separately and compare retrieved mixing ratios from each spectral region. Nadir observations of of the $\nu_{4}$ band probe the low stratosphere below 100 km. Our equatorial measurements at 289 cm$^{-1}$ show an abundance of (1.0$\pm$0.4) $\times$10$^{-5}$ at 88 km, from 2007 to 2017. This mixing ratio is consistent with measurements at higher altitudes, in contrast to the depletion that many photochemical models predict. Measurements from the $\nu_{12}$ and $\nu_{8}$ bands are comparable to each other, with the $\nu_{12}$ band probing an altitude range that extends deeper in the atmosphere. We suggest future studies of planetary atmospheres may observe the $\nu_{8}$ band, enabling shorter wavelength studies of ethane. There may also be an advantage to observing both the ethane $\nu_{8}$ band and nearby methane $\nu_{4}$ band in the same spectral window., Comment: 19 pages, 10 figures

From 2004 to 2017, the Cassini spacecraft orbited Saturn, completing 127 close flybys of its largest moon, Titan. Cassini's Composite Infrared Spectrometer (CIRS), one of 12 instruments carried on board, profiled Titan in the thermal infrared (7-1000 microns) throughout the entire 13-year mission. CIRS observed on both targeted encounters (flybys) and more distant opportunities, collecting 8.4 million spectra from 837 individual Titan observations over 3633 hours. Observations of multiple types were made throughout the mission, building up a vast mosaic picture of Titan's atmospheric state across spatial and temporal domains. This paper provides a guide to these observations, describing each type and chronicling its occurrences and global-seasonal coverage. The purpose is to provide a resource for future users of the CIRS data set, as well as those seeking to put existing CIRS publications into the overall context of the mission, and to facilitate future inter-comparison of CIRS results with those of other Cassini instruments, and ground-based observations., Comment: 62 pages, 31 figures, 10 tables. CSV format table data included

Observations of Neptune, made in 2018 using the new Narrow Field Adaptive Optics mode of the Multi Unit Spectroscopic Explorer (MUSE) instrument at the Very Large Telescope (VLT) from 0.48 - 0.93 micron, are analysed here to determine the latitudinal and vertical distribution of cloud opacity and methane abundance in Neptune's observable troposphere (0.1 - ~3 bar). Previous observations at these wavelengths in 2003 by HST/STIS (Karkoschka and Tomasko 2011, Icarus 205, 674-694) found that the mole fraction of methane above the cloud tops (at ~2 bar) varied from ~4% at equatorial latitudes to ~2% at southern polar latitudes, by comparing the observed reflectivity at wavelengths near 825 nm controlled primarily by either methane absorption or H2-H2/H2-He collision-induced absorption. We find a similar variation in cloud-top methane abundance in 2018, which suggests that this depletion of methane towards Neptune's pole is potentially a long-lived feature, indicative of long-term upwelling at mid-equatorial latitudes and subsidence near the poles. By analysing these MUSE observations along the central meridian with a retrieval model, we demonstrate that a broad boundary between the nominal and depleted methane abundances occurs at between 20 - 40S. We also find a small depletion of methane near the equator, perhaps indicating subsidence there, and a local enhancement near 60 - 70S, which we suggest may be associated with South Polar Features (SPFs) seen in Neptune's atmosphere at these latitudes. Finally, by the use of both a reflectivity analysis and a principal component analysis, we demonstrate that this depletion of methane towards the pole is apparent at all locations on Neptune's disc, and not just along its central meridian.

Recent analysis of Gemini-North/NIFS H-band (1.45 - 1.8 $\mu$m) observations of Uranus, recorded in 2010, with recently updated line data has revealed the spectral signature of hydrogen sulphide (H$_2$S) in Uranus's atmosphere (Irwin et al., 2018). Here, we extend this analysis to Gemini-North/NIFS observations of Neptune recorded in 2009 and find a similar detection of H$_2$S spectral absorption features in the 1.57 - 1.58 $\mu$m range, albeit slightly less evident, and retrieve a mole fraction of $\sim1-3$ ppm at the cloud tops. We find a much clearer detection (and much higher retrieved column abundance above the clouds) at southern polar latitudes compared with equatorial latitudes, which suggests a higher relative humidity of H$_2$S here. We find our retrieved H$_2$S abundances are most consistent with atmospheric models that have reduced methane abundance near Neptune's south pole, consistent with HST/STIS determinations (Karkoschka and Tomasko, 2011). We also conducted a Principal Component Analysis (PCA) of the Neptune and Uranus data and found that in the 1.57 - 1.60 $\mu$m range, some of the Empirical Orthogonal Functions (EOFs) mapped closely to physically significant quantities, with one being strongly correlated with the modelled H$_2$S signal and clearly mapping the spatial dependence of its spectral detectability. Just as for Uranus, the detection of H$_2$S at the cloud tops constrains the deep bulk sulphur/nitrogen abundance to exceed unity (i.e. $ > 4.4 - 5.0$ times the solar value) in Neptune's bulk atmosphere, provided that ammonia is not sequestered at great depths, and places a lower limit on its mole fraction below the observed cloud of (0.4 - 1.3) $\times 10^{-5}$. The detection of gaseous H$_2$S at these pressure levels adds to the weight of evidence that the principal constituent of the 2.5 - 3.5-bar cloud is likely to be H$_2$S ice., Comment: 13 Figures

We present sub-millimeter spectra of HCN isotopologues on Titan, derived from publicly available ALMA flux calibration observations of Titan taken in early 2014. We report the detection of a new HCN isotopologue on Titan, H$^{13}$C$^{15}$, and confirm an earlier report of detection of DCN. We model high signal-to-noise observations of HCN, H$^{13}$CN, HC$^{15}$N, DCN, and H$^{13}$C$^{15}$ to derive abundances and infer the following isotopic ratios: $^{12}$C/$^{13}$C = 89.8 $\pm$ 2.8, $^{14}$N/$^{15}$N = 72.3 $\pm$ 2.2, D/H = (2.5 $\pm$ 0.2)$\times$10$^{-4}$, and HCN/H$^{13}$C$^{15}$ = 5800 $\pm$ 270 (1$\sigma$ errors). The carbon and nitrogen ratios are consistent with and improve on the precision of previous results, confirming a factor of $\sim$2.3 elevation in $^{14}$N/$^{15}$N in HCN compared to N$_2$ and a lack of fractionation in $^{12}$C/$^{13}$C from the protosolar value. This is the first published measurement of D/H in a nitrile species on Titan, and we find evidence for a factor of $\sim$2 deuterium enrichment in hydrogen cyanide compared to methane. The isotopic ratios we derive may be used as constraints for future models to better understand the fractionation processes occurring in Titan's atmosphere., Comment: Accepted for publication in Astrophysical Journal Letters. 14 pages, 3 figures, 2 tables

We report interferometric observations of carbon monoxide (CO) and its isotopologues in Titan's atmosphere using the Atacama Large Millimeter/submillimeter Array (ALMA). The following transitions were detected: CO (J = 1-0, 2-1, 3-2, 6-5), $^{13}$CO (J = 2-1, 3-2, 6-5), C$^{18}$O (J = 2-1, 3-2), and C$^{17}$O (J = 3-2). Molecular abundances and the vertical atmospheric temperature profile were derived by modeling the observed emission line profiles using NEMESIS, a line-by-line radiative transfer code. We present the first spectroscopic detection of $^{17}$O in the outer solar system with C$^{17}$O detected at > 8$\sigma$ confidence. The abundance of CO was determined to be 49.6 ${\pm}$ 1.8 ppm, assumed to be constant with altitude, with isotopic ratios $^{12}$C/$^{13}$C = 89.9 ${\pm}$ 3.4, $^{16}$O/$^{18}$O = 486 ${\pm}$ 22, and $^{16}$O/$^{17}$O = 2917${\pm}$359. The measurements of $^{12}$C/$^{13}$C and $^{16}$O/$^{18}$O ratios are the most precise values obtained in Titan's atmospheric CO to date. Our results are in good agreement with previous studies and suggest no significant deviations from standard terrestrial isotopic ratios., Comment: Accepted for publication in ApJ Letters

The James Webb Space Telescope (JWST), scheduled for launch in 2018, is the successor to the Hubble Space Telescope (HST) but with a significantly larger aperture (6.5 m) and advanced instrumentation focusing on infrared science (0.6-28.0 $\mu$m ). In this paper we examine the potential for scientific investigation of Titan using JWST, primarily with three of the four instruments: NIRSpec, NIRCam and MIRI, noting that science with NIRISS will be complementary. Five core scientific themes are identified: (i) surface (ii) tropospheric clouds (iii) tropospheric gases (iv) stratospheric composition and (v) stratospheric hazes. We discuss each theme in depth, including the scientific purpose, capabilities and limitations of the instrument suite, and suggested observing schemes. We pay particular attention to saturation, which is a problem for all three instruments, but may be alleviated for NIRCam through use of selecting small sub-arrays of the detectors - sufficient to encompass Titan, but with significantly faster read-out times. We find that JWST has very significant potential for advancing Titan science, with a spectral resolution exceeding the Cassini instrument suite at near-infrared wavelengths, and a spatial resolution exceeding HST at the same wavelengths. In particular, JWST will be valuable for time-domain monitoring of Titan, given a five to ten year expected lifetime for the observatory, for example monitoring the seasonal appearance of clouds. JWST observations in the post-Cassini period will complement those of other large facilities such as HST, ALMA, SOFIA and next-generation ground-based telescopes (TMT, GMT, EELT)., Comment: 50 pages, including 22 figures and 2 tables

An extremely bright storm system observed in Uranus' atmosphere by amateur observers in September 2014 triggered an international campaign to observe this feature with many telescopes across the world. Observations of the storm system in the near infrared were acquired in October and November 2014 with SINFONI on ESO's Very Large Telescope (VLT) in Chile. SINFONI is an Integral Field Unit spectrometer returning 64x64 pixel images with 2048 wavelengths. Image cubes in the H-band (1.43 - 1.87 microns) were obtained at spatial resolutions of ~0.1". The observations show that the centre of the storm feature shifts markedly with increasing altitude, moving in the retrograde direction and slightly poleward with increasing altitude. We also see a faint 'tail' of more reflective material to the immediate south of the storm, which again trails in the retrograde direction. The observed spectra were analysed with the radiative transfer and retrieval code, NEMESIS. We find that the storm is well-modelled using either two main cloud layers of a 5-layer aerosol model based on Sromovsky et al. (2011) or by the simpler two-cloud-layer model of Tice et al. (2013). The deep component appears to be due to an increase in reflectivity and altitude of the main tropospheric cloud deck at 2 - 3 bars for both models, while the upper component of the feature was modelled as being due to either a thickening of the tropospheric haze of the 2-layer model or a vertical extension of the upper tropospheric cloud of the 5-layer model, assumed to be composed of methane ice and based at the methane condensation level at 1.23 bar. During the twelve days between our sets of observations the higher-altitude component of the feature was observed to have brightened significantly and extended to even higher altitudes, while the deeper component faded., Comment: 18 pages

Titan's middle atmosphere is currently experiencing a rapid change of season after northern spring arrived in 2009. A large cloud was observed for the first time above Titan's southern pole in May 2012, at an altitude of 300 km. This altitude previously showed a temperature maximum and condensation was not expected for any of Titan's atmospheric gases. Here we show that this cloud is composed of micron-sized hydrogen cyanide (HCN) ice particles. The presence of HCN particles at this altitude, together with new temperature determinations from mid-infrared observations, indicate a very dramatic cooling of Titan's atmosphere inside the winter polar vortex in early 2012. Such a cooling is completely contrary to previously measured high-altitude warming in the polar vortex, and temperatures are a hundred degrees colder than predicted by circulation models. Besides elucidating the nature of Titan's mysterious polar cloud, these results thus show that post-equinox cooling at the winter pole is much more efficient than previously thought., Comment: Published in Nature on 2 October 2014. This is the author version, before final editing by Nature

The Voyager 1 flyby of Titan in 1980 gave a first glimpse of the chemical complexity of Titan's atmosphere, detecting many new molecules with the infrared spectrometer (IRIS). These included propane (C3H8) and propyne (CH3C2H), while the intermediate-sized C3Hx hydrocarbon (C3H6) was curiously absent. Using spectra from the Composite Infrared Spectrometer (CIRS) on Cassini, we show the first positive detection of propene (C3H6) in Titan's stratosphere (5-sigma significance), finally filling the three-decade gap in the chemical sequence. We retrieve a vertical abundance profile from 100-250 km, that varies slowly with altitude from ~2 ppbv at 100 km, to ~5 ppbv at 200 km. The abundance of C3H6 is less than both C3H8 and CH3C2H, and we remark on an emerging paradigm in Titan's hydrocarbon abundances whereby: alkanes > alkynes > alkenes within the C2Hx and C3Hx chemical families in the lower stratosphere. More generally, there appears to be much greater ubiquity and relative abundance of triple-bonded species than double-bonded, likely due to the greater resistance of triple bonds to photolysis and chemical attack., Comment: 16 pages; 4 figures; 1 table. Withdrawn due to journal policy

In this chapter we describe the remote sensing measurement of nitrogen-bearing species in Titan's atmosphere by the Composite Infrared Spectrometer (CIRS) on the Cassini spacecraft. This instrument, which detects the thermal infrared spectrum from 10-1500 cm-1 (1000-7 microns) is sensitive to vibrational emissions of gases and condensates in Titan's stratosphere and lower mesosphere, permitting the measurement of ambient temperature and the abundances of gases and particulates. Three N-bearing species are firmly detected: HCN, HC3N and C2N2, and their vertical and latitudinal distributions have been mapped. In addition, ices of HC3N and possibly C4N2 are also seen in the far-infrared spectrum at high latitudes during the northern winter. The HC(15)N isotopologue has been measured, permitting the inference of the 14N/15N ratio in this species, which differs markedly (lower) than in the bulk nitrogen reservoir (N2). We also describe the search in the CIRS spectrum, and inferred upper limits, for NH3 and CH3CN. CIRS is now observing seasonal transition on Titan and the gas abundance distributions are changing accordingly, acting as tracers of the changing atmospheric circulation. The prospects for further CIRS science in the remaining five years of the Cassini mission are discussed., Comment: 19 pages, 9 figures, 1 table

In this paper we describe a first quantitative search for several molecules in Titan's stratosphere in Cassini CIRS infrared spectra. These are: ammonia (NH3), methanol (CH3OH), formaldehyde (H2CO), and acetonitrile (CH3CN), all of which are predicted by photochemical models but only the last of which observed, and not in the infrared. We find non-detections in all cases, but derive upper limits on the abundances from low-noise observations at 25{\deg}S and 75{\deg}N. Comparing these constraints to model predictions, we conclude that CIRS is highly unlikely to see NH3 or CH3OH emissions. However, CH3CN and H2CO are closer to CIRS detectability, and we suggest ways in which the sensitivity threshold may be lowered towards this goal., Comment: 11 pages plus 6 figure files

The flybys of Jupiter by the Voyager spacecraft in 1979, and over two decades later by Cassini in 2000, have provided us with unique datasets from two different epochs, allowing the investigation of seasonal change in the atmosphere. In this paper we model zonal averages of thermal infrared spectra from the two instruments, Voyager 1 IRIS and Cassini CIRS, to retrieve the vertical and meridional profiles of temperature, and the abundances of the two minor hydrocarbons, acetylene (C2H2) and ethane (C2H6). The spatial variation of these gases is controlled by both chemistry and dynamics, and therefore their observed distribution gives us an insight into both processes. We find that the two gases paint quite different pictures of seasonal change. Whilst the 2-D cross-section of C2H6 abundance is slightly increased and more symmetric in 2000 (northern summer solstice) compared to 1979 (northern fall equinox), the major trend of equator to pole increase remains. For C2H2 on the other hand, the Voyager epoch exhibits almost no latitudinal variation, whilst the Cassini era shows a marked decrease polewards in both hemispheres. At the present time, these experimental findings are in advance of interpretation, as there are no published models of 2-D Jovian seasonal chemical variation available for comparison., Comment: 48 pages, 12 figures, 5 tables

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