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Ethane Clathrate Hydrate Infrared Signatures for Solar System Remote Sensing E Dartois, F Langlet

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Ethane Clathrate Hydrate Infrared Signatures for Solar System Remote Sensing E Dartois, F Langlet Ethane clathrate hydrate infrared signatures for solar system remote sensing E Dartois, F Langlet To cite this version: E Dartois, F Langlet. Ethane clathrate hydrate infrared signatures for solar system remote sensing. Icarus, Elsevier, 2021. hal-03159998 HAL Id: hal-03159998 https://hal.archives-ouvertes.fr/hal-03159998 Submitted on 4 Mar 2021 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Ethane clathrate hydrate infrared signatures for solar system remote sensing. E. Dartois1, F. Langlet2, 1 Institut des Sciences Moléculaires d’Orsay, CNRS, Université Paris-Saclay, Bât 520, Rue André Rivière, 91405 Orsay, France e-mail: [email protected] 2 Institut d’Astrophysique Spatiale (IAS), UMR8617, CNRS, Université Paris-Saclay, Bât. 121, 91405 Orsay, France keywords: Planetary ices, IR spectroscopy, Clathrate hydrate, Ethane, Remote sensing To appear in Icarus Abstract their retention time scales in solar system bodies, and also mod- ify their release conditions. b=The hydrate term is sometimes Hydrocarbons such as methane and ethane are present in many used as a semantic shortcut to designate clathrate hydrates but solar system objects, including comets, moons and planets. The must not be confused neither with hydrates nor with ice mixtures interaction of these hydrocarbons with water ice at low temper- where a molecule is interacting with water ice and not necessar- atures could lead to the formation of inclusion compounds, such ily mediated via an ordered crystalline cage. as clathrate hydrates (water based host cages trapping hydrocar- Many models do include clathrate hydrates in the evolution bons guest molecules), modifying their retention, stability and or geophysical structure of solar system bodies, (e.g. Combe therefore evolution. The occurrence of =clathrate hydrates on b et al. 2019; Marounina et al. 2018; Castillo-Rogez et al. 2018; solar system surfaces could be established by remote sensing of Fu et al. 2017; Luspay-Kuti et al. 2016; Marboeuf et al. 2012). A their spectroscopic signatures. In this study, we measure and better understanding of clathrate kinetics and their spectroscopic analyse ethane clathrate hydrate spectra recorded in the temper- signatures is needed to continue addressing constraints on these ature range from 5.3 to 160K, covering most of the temperature clathrate hydrate models. A prerequisite for the identification of range of interest for solar system objects. Specific infrared band clathrate hydrates in the solar system is a thorough characterisa- signatures are identified for the ethane encaged guest. We pro- tion of the vibrational spectroscopic signatures in the infrared, or vide evidence that ethane clathrate hydrate outcrops can be de- the specific spectral fingerprints, and their evolution with the ice tected by remote sensing on the surface of planetary bodies. structure and temperature. For small guest molecules, clathrate hydrates can crystallise in two different cubic structures (I and 1. Introduction II), that will affect the filling of the ice cages and therefore the interactions and spectroscopy of the trapped species. Methane is Hydrocarbons are present in many solar system objects. The the main hydrocarbon found in cold solar system environments most abundant hydrocarbons species include gaseous methane b=(e.g. Glein and Zolotov 2020; Guzmán-Marmolejo and Segura or ethane present in the atmosphere of giant planets (e.g. Melin 2015, and citations above). Dedicated experiments (Dartois et al. et al. 2020; Guerlet et al. 2009; Sada et al. 1996; Tokunaga 2010; Dartois and Schmitt 2009; Dartois and Deboffle 2008, and et al. 1975), satellites atmospheres (Cours et al. 2020; Lom- references therein) have recorded the clathrate hydrate infrared bardo et al. 2019; Niemann et al. 2010), comets (Villanueva signatures in the 4K to 140K range, in the 2-4 µm (5000-2500 et al. 2011; Crovisier et al. 2004; Mumma et al. 2001, 2000), cm−1) range covering the fundamental stretching modes as well in the liquid b=phase on Titan (Farnsworth et al. 2019; Clark as the strongest combinations/overtones. et al. 2010; Cordier et al. 2009; Lunine and Atreya 2008), solid In addition to methane, ethane has been detected b=on Titan b=phase on Pluto and Triton (DeMeo et al. 2010), or Kuiper Belt and contributes to the hydrocarbon cycle (Brown et al. 2008; objects (Brown et al. 2007). The coexistence of hydrocarbons Mousis and Schmitt 2008; Barth and Toon 2006; Griffith et al. with water ice at low temperatures in some of these environ- 2006; Lunine et al. 1983). In some instances, such as the sur- ments b=raises the question about their ability to form clathrate face of Titan, the lower abundance of the ethane hydrocarbon hydrates. Clathrate hydrates are made of a 3-dimensional water- with respect to methane can be compensated by ethane’s lower molecule connected network, linked via hydrogen bonds. To vapour pressure, or its liquid state, and could favour the ethane be stabilized, the clathrate network hosts cavities encapsulating inclusion in the formation of clathrate hydrates. Missions target- guest molecules ("clathrate" meaning closure). Small molecules ing Titan, such as Dragonfly should better b=constrain the surface can be trapped in two main b=crystalline clathrate hydrate cubic and lower atmosphere conditions (e.g. Turtle et al. 2020; Voosen structures named type I and type II. The type I structure’s unit 12 2019; Lorenz et al. 2018). In this article we explore the infrared cell (e.g. Sloan and Koh 2007) is made of two dodecahedral (5 ) spectra of the ethane clathrate hydrate in the 5.3-160K range, water cages and six larger cages containing twelve pentagonal 12 2 and provide the spectroscopic signature and band frequencies of and two hexagonal faces (5 6 ) per unit cell. Another structure, the guest ethane trapped molecules. the type II structure, possesses sixteen dodecahedral (512) cages for eight large cages with twelve pentagonal and four hexagonal 12 4 faces (5 6 ) per unit cell. b=For each structure, the cage’s num- 2. Experiments ber ratio and the filling ratio with guest molecules influence the spectroscopic signatures of the trapped molecules. To form the ethane clathrate hydrate we followed a previously When the guests are relatively volatile species, like hydrocar- proven protocol in evacuated cryogenic cells (Dartois et al. 2010; bons such as methane and ethane, clathrate hydrates will modify Dartois and Schmitt 2009; Dartois and Deboffle 2008). The cell 1.0 0.8 0.6 0.4 Transmittance 0.2 0.0 4500 4000 3500 3000 2500 2000 1500 Wavenumber (cm-1) Fig. 1. Baseline corrected ethane clathrate hydrate transmittance spectrum recorded at 5.3K. Note the imperfect cancelation of the Fabry-Perot − fringes in the space between the ZnSe windows, leading to small waves observed superimposed on the b=spectrum (e.g. in the 2500-1700 cm 1 interval). Scattering effects deform the water ice bands because of imperfect film surface roughness once clathration is achieved. 20 K H O:C H 20:1 20 K H O:C H 20:1 1.5 2 2 6 1.5 2 2 6 15 K Cryst. C H 15 K Cryst. C H 2 6 2 6 11 12 11 * ν 8 ν ν + ν + + 6 12 7 5 8 4 11 8 6 ν ν ν ν ν , ν ν ν ν 1 + + ? ? ? + + 2 8 ν 2 6 ν ν ν 1.0 ν 1.0 * ** * 90 K C H /Oxirane Type I * * 90 K C H /Oxirane Type I 2 6 2 6 160 K 140 K 120 K 100 K 0.5 Optical depth + offset 0.5 Optical depth + offset 80 K 60 K 40 K 20 K 5.3 K 0.0 0.0 3000 2900 2800 2700 1500 1450 1400 1350 1300 1250 1200 Wavenumber (cm-1) Wavenumber (cm-1) Fig. 2. Temperature-dependent infrared spectra of the ethane clathrate in the fundamental modes regions. The crystalline pure ethane spectrum of Hudson et al. (2014) recorded at 15K is shown above. The infrared spectrum of an H2O:C2H6 (20:1) ice mixture from the Cosmic Ice Laboratory (Hudson et al., https://science.gsfc.nasa.gov/691/cosmicice/spectra.html), recorded at 20K, is shown above. The ethane:oxirane (7:3) mixed clathrate spectrum from Richardson et al. (1985) recorded at 90K is also shown. It is baseline corrected, and oxirane features are labelled with asterisks for clarity. Tentative assignments of the implied vibrational modes are given (see text for details). Spectra are offset for clarity. was built around two ZnSe windows facing each other, for in- The cell was pressurised with ethane gas at about 25 bars. This frared transmission analysis, sealed to an oxygen-free high ther- {pressure,temperature} couple is well above the stability curve mal conductivity (OFHC), gold coated, copper closed cell. It for ethane clathrate hydrate, which is about 3.5 bars at 267 K. was thermally coupled to a cold finger whose temperature can The system was kept under pressure b=for approximately fifteen be lowered using a liquid He transfer, balanced by a surrounding days, much above the expected diffusion kinetics time scale. If − Minco polyimide thermofoil heater, b=which maintains a con- one assumes a typical diffusion coefficient around 10 12m2=h at stant temperature. A high vacuum evacuated cryostat (P < 267K (e.g.
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