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14 results on '"Jean-Yves Bonnet"'

1. Influence of Calcium Perchlorate on the Search for Organics on Mars with Tetramethylammonium Hydroxide Thermochemolysis

Author

Yuanyuan He, Pin Lu, Paul R. Mahaffy, Charles Malespin, Melissa Guzman, Cyril Szopa, Amy J. Williams, Samuel Teinturier, Maeva Millan, Sarah Stewart Johnson, Michel Cabane, Hervé Cottin, Jennifer C. Stern, Jennifer L. Eigenbrode, Rafael Navarro-González, Vincent Butin, Fabien Stalport, Naila Chaouche-Mechidal, Caroline Freissinet, Arnaud Buch, D. Coscia, Daniel P. Glavin, Jamila El Bekri, Jean-Yves Bonnet, Laboratoire de Génie des Procédés et Matériaux (LGPM), CentraleSupélec-Université Paris-Saclay, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), University of Florida [Gainesville] (UF), NASA Goddard Space Flight Center (GSFC), Georgetown University [Washington] (GU), GSFC Solar System Exploration Division, Telespazio France, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Instituto de Ciencias Nucleares [Mexico], Universidad Nacional Autónoma de México = National Autonomous University of Mexico (UNAM), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Paris (UP)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12), and Universidad Nacional Autónoma de México (UNAM)

Subjects
chemistry.chemical_classification, Tetramethylammonium hydroxide, Perchlorates, Extraterrestrial Environment, Inorganic chemistry, Pyrolysis gc ms, Mars, Calcium perchlorate, Mars Exploration Program, 010402 general chemistry, 01 natural sciences, Agricultural and Biological Sciences (miscellaneous), Gas Chromatography-Mass Spectrometry, 0104 chemical sciences, Quaternary Ammonium Compounds, chemistry.chemical_compound, chemistry, [SDU]Sciences of the Universe [physics], 13. Climate action, Space and Planetary Science, 0103 physical sciences, Sample Analysis at Mars, Calcium, Organic matter, 010303 astronomy & astrophysics
Abstract

International audience; The Mars Organic Molecule Analyzer (MOMA) and Sample Analysis at Mars (SAM) instruments onboard the Exomars 2022 and Mars Science Laboratory rovers, respectively, are capable of organic matter detection and differentiating potentially biogenic from abiotic organics in martian samples. To identify organics, both these instruments utilize pyrolysis–gas chromatography coupled to mass spectrometry, and the thermochemolysis agent tetramethylammonium hydroxide (TMAH) is also used to increase organic volatility. However, the reactivity and efficiency of TMAH thermochemolysis are affected by the presence of calcium perchlorate on the martian surface. In this study, we determined the products of TMAH pyrolysis in the presence and absence of calcium perchlorate at different heating rates (flash pyrolysis and SAM-like ramp pyrolysis with a 35°C·min−1 heating rate). The decomposition mechanism of TMAH pyrolysis in the presence of calcium perchlorate was studied by using stepped pyrolysis. Moreover, the effect of calcium perchlorate (at Mars-relevant concentrations) on the recovery rate of fatty acids with TMAH thermochemolysis was studied. Results demonstrate that flash pyrolysis yields more diversity and greater abundances of TMAH thermochemolysis products than does the SAM-like ramp pyrolysis method. There is no obvious effect of calcium perchlorate on TMAH degradation when the [ClO4−] is lower than 10 weight percent (wt %). Most importantly, the presence of calcium perchlorate does not significantly impact the recovery rate of fatty acids with TMAH thermochemolysis under laboratory conditions, which is promising for the detection of fatty acids via TMAH thermochemolysis with the SAM and MOMA instruments on Mars.

Published
2021
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4. Influence of Calcium Perchlorate on the Search for Martian Organic Compounds with MTBSTFA/DMF Derivatization

Author

Sarah Stewart Johnson, Amy J. Williams, Daniel P. Glavin, Jean-Yves Bonnet, Melissa Guzman, Charles Malespin, Caroline Freissinet, Rafael Navarro-González, Michel Cabane, Arnaud Buch, Yuanyuan He, D. Coscia, Cyril Szopa, Maeva Millan, Jennifer L. Eigenbrode, Samuel Teinturier, Pin Lu, Paul R. Mahaffy, Laboratoire de Génie des Procédés et Matériaux (LGPM), CentraleSupélec-Université Paris-Saclay, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Department of Biology [Washington], Georgetown University [Washington] (GU), NASA Goddard Space Flight Center (GSFC), Instituto de Ciencias Nucleares [Mexico], Universidad Nacional Autónoma de México (UNAM), Department of Geological Sciences [Gainesville] (UF|Geological), University of Florida [Gainesville] (UF), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), and Telespazio France

Subjects
Extraterrestrial Environment, 010504 meteorology & atmospheric sciences, Inorganic chemistry, Mars, 01 natural sciences, Gas Chromatography-Mass Spectrometry, Perchlorate, chemistry.chemical_compound, 0103 physical sciences, Derivatization, 010303 astronomy & astrophysics, 0105 earth and related environmental sciences, Perchlorates, Chemistry, Chloromethane, Dimethylformamide, Calcium perchlorate, Agricultural and Biological Sciences (miscellaneous), 13. Climate action, Space and Planetary Science, Chlorobenzene, [SDU]Sciences of the Universe [physics], Reagent, Sample Analysis at Mars, Calcium, Pyrolysis
Abstract

International audience; N-tert-butyldimethylsilyl-N-methyltrifluoroacetamide (MTBSTFA), mixed with the solvent N,N-dimethylformamide (DMF), is used as a derivatizing reagent by the Sample Analysis at Mars (SAM) experiment onboard NASA's Curiosity rover and will soon be utilized by the Mars Organic Molecule Analyzer experiment onboard the ESA/Roscosmos Rosalind Franklin rover. The pyrolysis products of MTBSTFA, DMF, and the MTBSTFA/DMF mixtures, obtained at different temperatures, were analyzed. Two different pyrolysis modes were studied, flash pyrolysis and ramp pyrolysis (35°C/min), to evaluate the potential influence of the sample heating speed on the production of products in space chromatographs. The effect of the presence of calcium perchlorate on the pyrolysis products of MTBSTFA/DMF was also studied to ascertain the potential effect of perchlorate species known to be present at the martian surface. The results show that MTBSTFA/DMF derivatization should be applied below 300°C when using flash pyrolysis, as numerous products of MTBSTFA/DMF were formed at high pyrolysis temperatures. However, when an SAM-like ramp pyrolysis was applied, the final pyrolysis temperature did not appear to influence the degradation products of MTBSTFA/DMF. All products of MTBSTFA/DMF pyrolysis are listed in this article, providing a major database of products for the analysis of martian analog samples, meteorites, and the in situ analysis of martian rocks and soils. In addition, the presence of calcium perchlorate does not show any obvious effects on the pyrolysis of MTBSTFA/DMF: Only chloromethane and TBDMS-Cl (chloro-tertbutyldimethylsilane) were detected, whereas chlorobenzene and other chlorine-bearing compounds were not detected. However, other chlorine-bearing compounds were detected after pyrolysis of the Murchison meteorite in the presence of calcium perchlorate. This result reinforces previous suggestions that chloride-bearing compounds could be reaction products of martian samples and perchlorate.

Published
2021
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5. Molecular and isotopic behavior of insoluble organic matter of the Orgueil meteorite upon heating

Author

Laurent Remusat, Jean-Yves Bonnet, Sylvain Bernard, Eric Quirico, Arnaud Buch, Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), IMPEC - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Sorbonne Université (SU)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Sorbonne Université (SU), Institut de Planétologie et d'Astrophysique de Grenoble (IPAG), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG ), Institut polytechnique de Grenoble - Grenoble Institute of Technology [2007-2019] (Grenoble INP [2007-2019])-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology [2007-2019] (Grenoble INP [2007-2019])-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre National d'Études Spatiales [Toulouse] (CNES)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), and Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)

Subjects
010504 meteorology & atmospheric sciences, Hydrogen, Analytical chemistry, Orgueil, chemistry.chemical_element, 010502 geochemistry & geophysics, 01 natural sciences, Parent body, Geochemistry and Petrology, Chondrite, Insoluble organic matter, Organic matter, 0105 earth and related environmental sciences, chemistry.chemical_classification, Isotope, Carbonaceous chondrite, XANES, Isotopes of nitrogen, chemistry, Meteorite, 13. Climate action, [SDU]Sciences of the Universe [physics], D/H ratio, 15N/14N ratio, Hotspots
Abstract

International audience; Organic matter contained in carbonaceous chondrites may have evolved due to aqueous and/or thermal evolution on the parent body. The thermal behavior of the insoluble organic matter (IOM) of the Orgueil meteorite was investigated. The evolutions of structural and molecular properties were assessed by Raman, infrared and XANES spectroscopies, the H- and N-isotopic compositions by NanoSIMS. The starting IOM is a disordered organic macromolecule presenting a high degree of cross-linking. Hydrogen and Nitrogen isotope distributions are heterogeneous with the occurrence of numerous micron-sized hot spots enriched in heavy isotopes of H or N. After 1 hour at 300°C, there is subtle modification of the structural ordering and the isotopic compositions. After 1 hour at 500°C, the structure evolves toward condensation. Indeed, FTIR and XANES data are consistent with a continuous evolution of the molecular structure toward an increase of aromatization, starting at 300°C and becoming more intense at 500°C. The bulk D-enrichment is significantly reduced and D-rich hot spots are lost at 500°C. The experimental evolution of the δD is consistent with observations of IOM isolated from lightly altered carbonaceous chondrites. In contrast, the 15N-rich hot spots seem insensitive to high temperature up to 500°C and bulk δ15N remains constant. The thermal evolution of H- and N- isotopes is decoupled, indicating that the D-rich and 15N-rich moieties exhibit different thermal recalcitrance.

Published
2019
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6. Role of the Tenax® adsorbent in the interpretation of the EGA and GC‐MS analyses performed with the Sample Analysis at Mars in Gale crater

Author

Caroline Freissinet, Roger E. Summons, D. Coscia, Rafael Navarro-González, Daniel P. Glavin, Sarah Stewart Johnson, Imene Belmahdi, Cyril Szopa, Charles Malespin, Michel Cabane, Jennifer C. Stern, Paul R. Mahaffy, Jean-Yves Bonnet, Samuel Teinturier, Jennifer L. Eigenbrode, Maeva Millan, Yuanyuan He, Arnaud Buch, Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), NASA Goddard Space Flight Center (GSFC), Department of Earth, Atmospheric and Planetary Sciences [MIT, Cambridge] (EAPS), Massachusetts Institute of Technology (MIT), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Instituto de Ciencias Nucleares [Mexico], Universidad Nacional Autónoma de México (UNAM), and Georgetown University [Washington] (GU)

Subjects
010504 meteorology & atmospheric sciences, Tenax, Martian soil, Mars Exploration Program, 01 natural sciences, chemistry.chemical_compound, Perchlorate, Geophysics, chemistry, 13. Climate action, Space and Planetary Science, Geochemistry and Petrology, [SDU]Sciences of the Universe [physics], Reagent, Environmental chemistry, Sample Analysis at Mars, Earth and Planetary Sciences (miscellaneous), Gas chromatography–mass spectrometry, Derivatization, 0105 earth and related environmental sciences
Abstract

The Sample Analysis at Mars (SAM) experiment on the National Aeronautics and Space Administration Curiosity rover seeks evidence of organic compounds on the surface of Mars. Since the beginning of the mission, various organic molecules have been detected and identified. While several have been demonstrated to be indigenous to the Martian soil and rocks analyzed, others appear to have been produced from sources internal to the experiment. The objective of this study is to build an exhaustive molecular database to support the interpretation of SAM results by identifying all the chemical species produced from Tenax® adsorbents, by determining (1) the thermal degradation by‐products of Tenax®, (2) the effect of Tenax® conditioning on the formation of Tenax® by‐products, (3) the impact of MTBSTFA or a mixture of MTBSTFA and DMF on Tenax® decomposition, and (4) the reaction between Tenax® and calcium perchlorate. Our results indicate that the by‐products of the SAM trap are due to the impact of trap heating, the impact of the derivatization reagent (MTBSTFA) and the presence of perchlorate in Martian soil. Some of these by‐products are observed in the SAM gas chromatograph mass spectrometer data from Mars.

Published
2019
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7. Application of TMAH thermochemolysis to the detection of nucleobases: Application to the MOMA and SAM space experiment

Author

Pin Lu, Paul R. Mahaffy, M. Morisson, Cyril Szopa, Melissa Guzman, Jason P. Dworkin, Maeva Millan, J. L. Eigenbrode, Jean-Yves Bonnet, Caroline Freissinet, Sarah Stewart Johnson, Amy J. Williams, Yuanyuan He, D. Coscia, Arnaud Buch, Daniel P. Glavin, Charles Malespin, Rafael Navarro-González, Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), University of Florida [Gainesville] (UF), Georgetown University [Washington] (GU), NASA Goddard Space Flight Center (GSFC), Laboratorio de Química de Plasmas y Estudios Planetarios [Mexico], Instituto de Ciencias Nucleares [Mexico], Universidad Nacional Autónoma de México (UNAM)-Universidad Nacional Autónoma de México (UNAM), Telespazio France, and Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)

Subjects
Hot Temperature, Guanine, Mars, MOMA, 02 engineering and technology, Pyrimidinones, 01 natural sciences, Gas Chromatography-Mass Spectrometry, Analytical Chemistry, Nucleobase, chemistry.chemical_compound, Limit of Detection, Hypoxanthine, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Tetramethylammonium hydroxide, Nucleobases, Chromatography, Tetramethylammonium hydroxide (TMAH)SAM, 010401 analytical chemistry, Uracil, Space Flight, 021001 nanoscience & nanotechnology, Derivatization, 0104 chemical sciences, Thymine, chemistry, 13. Climate action, Purines, Sample Analysis at Mars, Thermochemolysis, GC-MS, 0210 nano-technology, Cytosine, Pyrolysis
Abstract

International audience; Thermochemolysis of seven nucleobases—adenine, thymine, uracil, cytosine, guanine, xanthine, and hypoxanthine—in tetramethylammonium hydroxide (TMAH) was studied individually by pyrolysis gas chromatography mass spectrometry in the frame of the Mars surface exploration. The analyses were performed under conditions relevant to the Sample Analysis at Mars (SAM) instrument of the Mars Curiosity Rover and the Mars Organic Molecule Analyzer (MOMA) instrument of the ExoMars Rover. The thermochemolysis products of each nucleobase were identified and the reaction mechanisms studied. The thermochemolysis temperature was optimized and the limit of detection and quantification of each nucleobase were also investigated. Results indicate that 600°C is the optimal thermochemolysis temperature for all seven nucleobases. The methylated products trimethyl-adenine, 1, 3-dimethyl-thymine, 1, 3-dimethyl-uracil, trimethyl-cytosine, 1, 3, 7-trimethyl-xanthine (caffeine), and dimethyl-hypoxanthine, respectively, are the most stable forms of adenine, thymine, uracil, cytosine, guanine, and xanthine, and hypoxanthine in TMAH solutions. The limits of detection for adenine, thymine, and uracil were 0.075 nmol; the limits of detection for guanine, cytosine, and hypoxanthine were higher, at 0.40, 0.55, and 0.75 nmol, respectively. These experiments allowed to well constrain the analytical capabilities of the thermochemolysis experiments that will be performed on Mars to detect nucleobases.

Published
2019
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8. Operations of the Sample Analysis at Mars instrument suite onboard the Curiosity rover

Author

Caroline Freissinet, Arnaud Buch, Samuel Teinturier, Micah Johnson, Jean-Yves Bonnet, Eric Lorigny, Cyril Szopa, Michel Cabane, Paul R. Mahaffy, Mehdi Benna, Charles Malespin, Stephen Indyk, David Coscia, B. D. Prats, Laboratoire Atmosphères, Milieux, Observations Spatiales ( LATMOS ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Telespazio France, IMPEC - LATMOS, Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ) -Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), CentraleSupélec, Honeybee Robotics Ltd, NASA Goddard Space Flight Center ( GSFC ), eINFORMe inc., Centre National d'Etudes Spatiales ( CNES ), Goddard Earth Sciences and Technology and Research ( GESTAR ), Universities Space Research Association ( USRA ) -NASA, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), PLANETO - LATMOS, Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS), Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), NASA Goddard Space Flight Center (GSFC), Centre National d'Études Spatiales [Toulouse] (CNES), Goddard Earth Sciences and Technology and Research (GESTAR), and Universities Space Research Association (USRA)-NASA

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Martian, Scientific instrument, Engineering, [SDU.ASTR]Sciences of the Universe [physics]/Astrophysics [astro-ph], 010504 meteorology & atmospheric sciences, Spectrometer, business.industry, Payload, Suite, Mars Exploration Program, 01 natural sciences, Workflow, [ PHYS.PHYS.PHYS-AO-PH ] Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], 0103 physical sciences, Sample Analysis at Mars, Aerospace engineering, business, 010303 astronomy & astrophysics, [ SDU.ASTR ] Sciences of the Universe [physics]/Astrophysics [astro-ph], 0105 earth and related environmental sciences
Abstract

The Sample Analysis at Mars instrument suite, onboard the Curiosity rover, has been analyzing the martian environment since August 05th 2012, as one of the main tools of the Mars Science Laboratory mission. This suite is composed of three independent but interoperable instruments, namely a Quadrupole Mass Spectrometer, a Tunable Laser Spectrometer and a Gas Chromatograph, plus a sophisticated Sample Manipulation System. SAM is used to analyze soils, rocks and atmosphere. For instance, it detected in situ martian complex organics for the first time, provide us with a several years survey of the atmospheric composition and helped understand how the martian environment evolved through the planet history. At 40 kg, it represents half of the scientific payload weight of Curiosity and is one of the two analytical instruments of the mission. This instrument suite is the result of an international collaboration between the NASA Goddard Space Flight Center, the NASA Jet Propulsion Laboratory and a consortium of French laboratories supported by the Center National d’Etudes Spatiales (the French space agency). This contribution will present the organization of the SAM operational workflow from the ground infrastructure, to flight operations and laboratory supporting work. It will also describe how the CNES hosts and supports the SAM team during this exciting mission.

Published
2018
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9. Compositional and structural investigation of HCN polymer through high resolution mass spectrometry

Author

Roland Thissen, Roger V. Yelle, Odile Dutuit, Eric Quirico, François-Régis Orthous-Daunay, Jean-Yves Bonnet, Sarah M. Hörst, Véronique Vuitton, Hervé Cottin, Léna Le Roy, Nicolas Fray, and Maeliss Frisari

Subjects
chemistry.chemical_classification, Collision-induced dissociation, Infrared, Chemistry, Analytical chemistry, Aromaticity, Polymer, 010402 general chemistry, Condensed Matter Physics, Mass spectrometry, 01 natural sciences, 0104 chemical sciences, Elemental analysis, 0103 physical sciences, Mass spectrum, Physical and Theoretical Chemistry, Spectroscopy, 010303 astronomy & astrophysics, Instrumentation
Abstract

Nitrogen rich compounds are found in numerous planetary environments such as planetary atmospheres, meteorites and comets. To better understand the structure and composition of this natural organic material, laboratory analogs have been studied. Though HCN polymers have been studied since the beginning of the 19th century, their structure and composition are still poorly understood. In this work we report the first extended high resolution mass spectrometry study of HCN polymers. The mass spectra of the polymer contain hundreds of peaks to which we try to assign an elemental composition. Elemental analysis has been used to constrain the molecular formulae and isotopic signatures have also been used to confirm them. The large quantity of amine functions observed with both infrared (IR) spectroscopy and mass spectrometry indicates that amine groups are present in most chains found in HCN polymer. Collision induced dissociation (CID) tandem (MSn) measurements were also performed on eight molecular ions and aromatic rings have been identified.

Published
2013
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10. In situ analysis of martian regolith with the SAM experiment during the first mars year of the MSL mission: Identification of organic molecules by gas chromatography from laboratory measurements

Author

Arnaud Buch, Maeva Millan, Cyril Szopa, Paul R. Mahaffy, Samuel Teinturier, Michel Cabane, Jean-Yves Bonnet, Patrice Coll, D. Coscia, Daniel P. Glavin, Caroline Freissinet, Pascaline Francois, Rafael Navarro-González, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), NASA Goddard Space Flight Center (GSFC), Center for Space Sciences and Technology (CSST), University of Maryland [Baltimore County] (UMBC), University of Maryland System-University of Maryland System, Instituto de Ciencias Nucleares [Mexico], Universidad Nacional Autónoma de México (UNAM), Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Poitiers-Institut de Chimie du CNRS (INC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre National d'Etudes Spatiales (CNES), Universidad Nacional Autónoma de México = National Autonomous University of Mexico (UNAM), Université de Poitiers-Institut national des sciences de l'Univers (INSU - CNRS)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), IMPEC - LATMOS, Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Center for Space Science and Technology (CSST), and Université de Poitiers-Centre National de la Recherche Scientifique (CNRS)

Subjects
Martian, 010504 meteorology & atmospheric sciences, [SDU.ASTR.EP]Sciences of the Universe [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], Astronomy and Astrophysics, Martian soil, Mars Exploration Program, Mass spectrometry, 01 natural sciences, Regolith, Astrobiology, [SDU.ASTR.IM]Sciences of the Universe [physics]/Astrophysics [astro-ph]/Instrumentation and Methods for Astrophysic [astro-ph.IM], 13. Climate action, Space and Planetary Science, Martian surface, 0103 physical sciences, Sample Analysis at Mars, Environmental science, Gas chromatography–mass spectrometry, 010303 astronomy & astrophysics, 0105 earth and related environmental sciences
Abstract

International audience; The Sample Analysis at Mars (SAM) instrument onboard the Curiosity rover, is specifically designed for in situ molecular and isotopic analyses of martian surface materials and atmosphere. It contributes to the Mars Science Laboratory (MSL) missions primary scientific goal to characterize the potential past, present or future habitability of Mars. In all of the analyses of solid samples delivered to SAM so far, chlorinated organic compounds have been detected above instrument background levels and identified by gas chromatography coupled to mass spectrometry (GC–MS) (Freissinet et al., 2015; Glavin et al., 2013). While some of these may originate from reactions between oxychlorines and terrestrial organic carbon present in the instrument background (Glavin et al., 2013), others have been demonstrated to originate from indigenous organic carbon present in samples (Freissinet et al., 2015).We present here laboratory calibrations that focused on the analyses performed with the MXT-CLP GC column (SAM GC-5 channel) used for nearly all of the GC–MS analyses of the martian soil samples carried out with SAM to date. Complementary to the mass spectrometric data, gas chromatography allows us to separate and identify the species analyzable in a nominal SAM-GC run time of about 21 min. To characterize the analytical capabilities of this channel within the SAM Flight Model (FM) operating conditions on Mars, and their implications on the detection of organic matter, it is required to perform laboratory experimental tests and calibrations on spare model components. This work assesses the SAM flight GC-5 column efficiency, confirms the identification of the molecules based on their retention time, and enables a better understanding of the behavior of the SAM injection trap (IT) and its release of organic molecules. This work will enable further optimization of the SAM-GC runs for additional samples to be analyzed during the MSL mission.

Published
2016
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11. Formation of analogs of cometary nitrogen-rich refractory organics from thermal degradation of tholin and hcn polymer

Author

Emmanuel Dartois, Nathalie Carrasco, Léna Le Roy, Arnaud Buch, Roland Thissen, Nicolas Fray, Jean-Yves Bonnet, Rosario Brunetto, Gilles Montagnac, Cécile Engrand, Eric Quirico, Guy Cernogora, J. Duprat, Hervé Cottin, Cyril Szopa, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Planétologie et d'Astrophysique de Grenoble (IPAG), Centre National d'Études Spatiales [Toulouse] (CNES)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, IMPEC - LATMOS, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement [Lyon] (LGL-TPE), École normale supérieure - Lyon (ENS Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut d'astrophysique spatiale (IAS), Université Paris-Sud - Paris 11 (UP11)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre de Spectrométrie Nucléaire et de Spectrométrie de Masse (CSNSM), Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), Institut de Planétologie et d'Astrophysique de Grenoble (IPAG ), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), PLANETO - LATMOS, Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement (LGL-TPE), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet - Saint-Étienne (UJM)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Sud - Paris 11 (UP11)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Université Paris-Sud - Paris 11 (UP11), Laboratoire Atmosphères, Milieux, Observations Spatiales ( LATMOS ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Institut de Planétologie et d'Astrophysique de Grenoble ( IPAG ), Observatoire des Sciences de l'Univers de Grenoble ( OSUG ), Université Joseph Fourier - Grenoble 1 ( UJF ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ) -Université Grenoble Alpes ( UGA ) -Université Joseph Fourier - Grenoble 1 ( UJF ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ) -Université Grenoble Alpes ( UGA ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire de Génie des Procédés et Matériaux - EA 4038 ( LGPM ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ) -Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Institut Universitaire de France ( IUF ), Ministère de l'Éducation nationale, de l’Enseignement supérieur et de la Recherche ( M.E.N.E.S.R. ), Laboratoire inter-universitaire des systèmes atmosphèriques ( LISA ), Institut national des sciences de l'Univers ( INSU - CNRS ) -Université Paris Diderot - Paris 7 ( UPD7 ) -Université Paris-Est Créteil Val-de-Marne - Paris 12 ( UPEC UP12 ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement [Lyon] ( LGL-TPE ), École normale supérieure - Lyon ( ENS Lyon ) -Université Claude Bernard Lyon 1 ( UCBL ), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Institut d'astrophysique spatiale ( IAS ), Université Paris-Sud - Paris 11 ( UP11 ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Centre de Spectrométrie Nucléaire et de Spectrométrie de Masse ( CSNSM ), Université Paris-Sud - Paris 11 ( UP11 ) -Institut National de Physique Nucléaire et de Physique des Particules du CNRS ( IN2P3 ) -Centre National de la Recherche Scientifique ( CNRS ), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], education.field_of_study, Carbonization, Population, chemistry.chemical_element, Organic chemistry, Astronomy and Astrophysics, Tholin, Photochemistry, Astrobiology, Cosmochemistry, [ PHYS.PHYS.PHYS-AO-PH ] Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], chemistry, 13. Climate action, Space and Planetary Science, Interplanetary dust, Comets, Solar nebula, Meteoritics, education, Carbon, Chemical composition, Refractory (planetary science)
Abstract

International audience; Nitrogen-rich refractory organics are scarce phases recovered as a fraction of stratospheric IDPs and constitute the bulk of the organic matter of some ultracarbonaceous Antarctic micrometeorites. They are likely formed under very specific conditions within a nitrogen-rich environment and may provide valuable clues on the origin of the population of interplanetary dusts accreted by Earth. In this study, we produced relevant analogs of such refractory organics characterized in three ultracarbonaceous Antarctic micrometeorites, starting from the carbonization of an HCN polymer and a tholin. Indeed, carbonization is a process that can increase the polyaromatic character toward a structure similar to that observed in these cosmomaterials. Both these precursors were degraded in an Ar atmosphere at 300, 500, 700 and 1000°C over ∼1 hour and characterized by elemental analysis, micro-FTIR and Raman micro-spectroscopy (at 244 and 514 nm excitation wavelengths). Our results show that the precursors evolve along distinct chemical and structural pathways during carbonization and that the influence of the precursor structure is still very strong at 1000°C. Interestingly, these different carbonization routes appear in the spectral characteristics of the G and D bands of their Raman spectra. Several of the residues present chemical and structural similarities with three recently studied ultracarbonaceous micrometeorites [Dobrica et al. (2011)Meteoritics Planet. Sci.46, 1363; Dartois et al. (2013)Icarus224, 243] and with N-rich inclusions in stratospheric IDPs. However the residues do not simultaneously account for the carbon structure (Raman) and the chemical composition (IR, N/C ratio). This indicates that the precursors and/or heating conditions in our experiments are not fully relevant. Despite this lack of full relevancy, the formation of a polyaromatic structure fairly similar to that of UCAMMs and IDPs suggests that the origin of N-rich refractory organics lies in a thermal process in the proto-solar disk, however radiolysis cannot be excluded.

Published
2015
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12. Very high resolution mass spectrometry of HCN polymers and tholins

Author

Nathalie Carrasco, Bernard Schmitt, Hervé Cottin, Roland Thissen, Léna Le Roy, Odile Dutuit, Jean-Yves Bonnet, Véronique Vuitton, Eric Quirico, Ella Sciamma-O'Brien, Cyril Szopa, Nicolas Fray, Maeliss Frisari, Laboratoire de Planétologie de Grenoble (LPG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique et chimie de l'environnement (LPCE), Université d'Orléans (UO)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Planétologie de Grenoble ( LPG ), Université Joseph Fourier - Grenoble 1 ( UJF ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire de physique et chimie de l'environnement ( LPCE ), Institut national des sciences de l'Univers ( INSU - CNRS ) -Université d'Orléans ( UO ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire inter-universitaire des systèmes atmosphèriques ( LISA ), Institut national des sciences de l'Univers ( INSU - CNRS ) -Université Paris Diderot - Paris 7 ( UPD7 ) -Université Paris-Est Créteil Val-de-Marne - Paris 12 ( UPEC UP12 ) -Centre National de la Recherche Scientifique ( CNRS ), IMPEC - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales ( LATMOS ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ) -Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Centre National de la Recherche Scientifique ( CNRS ), Institut national des sciences de l'Univers (INSU - CNRS)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, 010504 meteorology & atmospheric sciences, [PHYS.ASTR.EP]Physics [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], Analytical chemistry, [SDU.ASTR.EP]Sciences of the Universe [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], Infrared spectroscopy, Tholin, Polymer, Mass spectrometry, 01 natural sciences, [ SDU.ASTR.EP ] Sciences of the Universe [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], chemistry, Polymerization, [ PHYS.ASTR.EP ] Physics [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], 13. Climate action, Elemental analysis, 0103 physical sciences, Molecule, Physical and Theoretical Chemistry, 010303 astronomy & astrophysics, Chemical composition, 0105 earth and related environmental sciences
Abstract

International audience; HCN polymers are complex organic solids resulting from the polymerization of hydrogen cyanide (HCN) molecules. They have been suspected to contribute to the refractory carbonaceous component of comets as well as the distributed CN sources in cometary atmospheres. Titan's tholins are also organic compounds produced in a laboratory setting but result from the complex chemistry between N2 and CH4 induced by UV radiation or electric discharges. Some of these compounds have optical properties in the visible range fairly similar to those of Titan's aerosols or those of the reddish surfaces of many icy satellites and small bodies. It has been proposed that HCN polymers are constituents of tholins but this statement has never received any clear demonstration. We report here on the comparative analysis of tholins and HCN polymers in order to definitely establish if the molecules identified in the HCN polymers are present in the tholins as well. First, we present a global comparison of HCN polymers with three kinds of tholins, using elemental analysis measurements, infrared spectroscopy and very high resolution mass spectrometry of their soluble fraction. We show that the chemical composition of the HCN polymers is definitely simpler than that of any of the tholins studied. Second, we focus on six ions representative of the composition of HCN polymers and using mass spectrometry (HRMS and MS/HRMS), we determine that these tholins contain at best a minor fraction of this kind of HCN polymers.

Published
2010
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13. Chemical characterization of Titan's tholins: solubility, morphology and molecular structure revisited

Author

Odile Dutuit, Olivier Laprévote, Guy Cernogora, Gilles Adandé, Isabelle Schmitz-Afonso, Roland Thissen, Cyril Szopa, Arnaud Buch, Jean-Yves Bonnet, Edith Hadamcik, Fakhreddine Ouni, Nathalie Carrasco, Eric Quirico, Aïcha Bagag, Alexandre Giulani, PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie des Substances Naturelles (ICSN), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire de Planétologie de Grenoble (LPG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Génie des Procédés et Matériaux - EA 4038 (LGPM), CentraleSupélec, and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
010504 meteorology & atmospheric sciences, Extraterrestrial Environment, Spectrophotometry, Infrared, [PHYS.ASTR.EP]Physics [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], Nitrogen, Analytical chemistry, [SDU.ASTR.EP]Sciences of the Universe [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], Infrared spectroscopy, Mass spectrometry, 01 natural sciences, Methane, Mass Spectrometry, chemistry.chemical_compound, symbols.namesake, thermodynamics, gas, 0103 physical sciences, Physical and Theoretical Chemistry, Solubility, Particle Size, 010303 astronomy & astrophysics, plasma, 0105 earth and related environmental sciences, Molecular Structure, Chemistry, Atmosphere, Methanol, Tholin, mass-spectrometry, simulation, atmospheric-pressure photoionization, high polymer-solutions, haze, Solvent, Atmospheric Pressure, Saturn, Atmospheric chemistry, symbols, Microscopy, Electron, Scanning, Solvents, Titan (rocket family), Porosity
Abstract

In this work Titan's atmospheric chemistry is simulated using a capacitively coupled plasma radio frequency discharge in a N(2)-CH(4) stationnary flux. Samples of Titan's tholins are produced in gaseous mixtures containing either 2 or 10% methane before the plasma discharge, covering the methane concentration range measured in Titan's atmosphere. We study their solubility and associated morphology, their infrared spectroscopy signature and the mass distribution of the soluble fraction by mass spectrometry. An important result is to highlight that the previous Titan's tholin solubility studies are inappropriate to fully characterize such a heterogeneous organic matter and we develop a new protocol to evaluate quantitatively tholins solubility. We find that tholins contain up to 35% in mass of molecules soluble in methanol, attached to a hardly insoluble fraction. Methanol is then chosen as a discriminating solvent to characterize the differences between soluble and insoluble species constituting the bulk tholins. No significant morphological change of shape or surface feature is derived from scanning electron microscopy after the extraction of the soluble fraction. This observation suggests a solid structure despite an important porosity of the grains. Infrared spectroscopy is recorded for both fractions. The IR spectra of the bulk, soluble, and insoluble tholins fractions are found to be very similar and reveal identical chemical signatures of nitrogen bearing functions and aliphatic groups. This result confirms that the chemical information collected when analyzing only the soluble fraction provides a valuable insight representative of the bulk material. The soluble fraction is ionized with an atmospheric pressure photoionization source and analyzed by a hybrid mass spectrometer. The congested mass spectra with one peak at every mass unit between 50 and 800 u confirm that the soluble fraction contains a complex mixture of organic molecules. The broad distribution, however, exhibits a regular pattern of mass clusters. Tandem collision induced dissociation analysis is performed in the negative ion mode to retrieve structural information. It reveals that (i) the molecules are ended by methyl, amine and cyanide groups, (ii) a 27 u neutral moiety (most probably HCN) is often released in the fragmentation of tholin anions, and (iii) an ubiquitous ionic fragment at m/z 66 is found in all tandem spectra. A tentative structure is proposed for this negative ion.

Published
2009
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14. Very high resolution mass spectrometry of HCN polymers and tholins.

Author

Véronique Vuitton, Jean-Yves Bonnet, Maeliss Frisari, Roland Thissen, Eric Quirico, Odile Dutuit, Bernard Schmitt, Léna Le Roy, Nicolas Fray, Hervé Cottin, Ella Sciamma-O'Brien, Nathalie Carrasco, and Cyril Szopa

Abstract

HCN polymers are complex organic solids resulting from the polymerization of hydrogen cyanide (HCN) molecules. They have been suspected to contribute to the refractory carbonaceous component of comets as well as the distributed CN sources in cometary atmospheres. Titan's tholins are also organic compounds produced in a laboratory setting but result from the complex chemistry between N2and CH4induced by UV radiation or electric discharges. Some of these compounds have optical properties in the visible range fairly similar to those of Titan's aerosols or those of the reddish surfaces of many icy satellites and small bodies. It has been proposed that HCN polymers are constituents of tholins but this statement has never received any clear demonstration. We report here on the comparative analysis of tholins and HCN polymers in order to definitely establish if the molecules identified in the HCN polymers are present in the tholins as well. First, we present a global comparison of HCN polymers with three kinds of tholins, using elemental analysis measurements, infrared spectroscopy and very high resolution mass spectrometry of their soluble fraction. We show that the chemical composition of the HCN polymers is definitely simpler than that of any of the tholins studied. Second, we focus on six ions representative of the composition of HCN polymers and using mass spectrometry (HRMS and MS/HRMS), we determine that these tholins contain at best a minor fraction of this kind of HCN polymers. [ABSTRACT FROM AUTHOR]

Published
2010
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