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Nitrogen incorporation in Titan's tholins inferred by high resolution orbitrap mass spectrometry and gas chromatography–mass spectrometry
Influx of solar photons and heavy charged particles from Saturn's magnetosphere on Titan's atmosphere – mainly comprised of methane and nitrogen – induce an intense organic photochemistry which leads to the formation of a large amount of aerosols in suspension in the atmosphere. In order t...
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Published in: | Earth and planetary science letters 2014-10, Vol.404, p.33-42 |
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creator | Gautier, Thomas Carrasco, Nathalie Schmitz-Afonso, Isabelle Touboul, David Szopa, Cyril Buch, Arnaud Pernot, Pascal |
description | Influx of solar photons and heavy charged particles from Saturn's magnetosphere on Titan's atmosphere – mainly comprised of methane and nitrogen – induce an intense organic photochemistry which leads to the formation of a large amount of aerosols in suspension in the atmosphere. In order to infer the role of nitrogen in aerosol formation processes we produced laboratory analogs of Titan's aerosols. In this work, we compare the composition of different analogs by using high resolution mass spectrometry and propose an additional study using gas-chromatography coupled to mass-spectrometry for a new kind of analog produced by polymerization of cryogenically trapped gaseous neutral species. The comparison of these materials emphasizes the importance of ion chemistry processes for the inclusion of nitrogen in molecules constituting Titan's tholins. A statistical approach is also used for the treatment of high resolution mass spectra of these highly complex organic materials. This method allows distinguishing molecular families that can be reconstructed by an ideal copolymer. We investigate several copolymer reconstructions, and we suggest that an HCN (or CH3CN)/C2H4 based copolymer agrees well with the polymeric structure of tholins produced with 5% of methane in nitrogen.
•We analyze different Titan's tholins with orbitrap mass spectrometry.•Results show the importance of ionic chemistry for nitrogen incorporation in tholins.•A statistical approach is used to deal with the high complexity of the mass spectra.•Tholins structures present different molecular families.•Copolymer reconstruction suggests HCN/C2H4 as a possible pattern for polymerization. |
doi_str_mv | 10.1016/j.epsl.2014.07.011 |
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•We analyze different Titan's tholins with orbitrap mass spectrometry.•Results show the importance of ionic chemistry for nitrogen incorporation in tholins.•A statistical approach is used to deal with the high complexity of the mass spectra.•Tholins structures present different molecular families.•Copolymer reconstruction suggests HCN/C2H4 as a possible pattern for polymerization.</description><identifier>ISSN: 0012-821X</identifier><identifier>EISSN: 1385-013X</identifier><identifier>DOI: 10.1016/j.epsl.2014.07.011</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>Aerosols ; Analogs ; Astrophysics ; Atmospheric and Oceanic Physics ; Copolymers ; Earth and Planetary Astrophysics ; High resolution ; high resolution mass spectrometry ; Mass spectrometry ; Methane ; nitrogen ; Physics ; Saturn satellites ; Sciences of the Universe ; tholins ; Titan ; Titan's atmosphere</subject><ispartof>Earth and planetary science letters, 2014-10, Vol.404, p.33-42</ispartof><rights>2014 Elsevier B.V.</rights><rights>Attribution - NonCommercial</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a533t-1e4763dca963db21bc61d07b691cafcba76d2ce73d22e33cd666566184d771d13</citedby><cites>FETCH-LOGICAL-a533t-1e4763dca963db21bc61d07b691cafcba76d2ce73d22e33cd666566184d771d13</cites><orcidid>0000-0002-0090-4056 ; 0000-0002-0596-6336 ; 0000-0002-9794-5056 ; 0000-0002-2097-7252 ; 0000-0003-2751-774X ; 0000-0001-8586-6222 ; 0000-0003-0665-0074</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,780,784,885,27924,27925</link.rule.ids><backlink>$$Uhttps://hal.science/hal-01056129$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Gautier, Thomas</creatorcontrib><creatorcontrib>Carrasco, Nathalie</creatorcontrib><creatorcontrib>Schmitz-Afonso, Isabelle</creatorcontrib><creatorcontrib>Touboul, David</creatorcontrib><creatorcontrib>Szopa, Cyril</creatorcontrib><creatorcontrib>Buch, Arnaud</creatorcontrib><creatorcontrib>Pernot, Pascal</creatorcontrib><title>Nitrogen incorporation in Titan's tholins inferred by high resolution orbitrap mass spectrometry and gas chromatography–mass spectrometry</title><title>Earth and planetary science letters</title><description>Influx of solar photons and heavy charged particles from Saturn's magnetosphere on Titan's atmosphere – mainly comprised of methane and nitrogen – induce an intense organic photochemistry which leads to the formation of a large amount of aerosols in suspension in the atmosphere. In order to infer the role of nitrogen in aerosol formation processes we produced laboratory analogs of Titan's aerosols. In this work, we compare the composition of different analogs by using high resolution mass spectrometry and propose an additional study using gas-chromatography coupled to mass-spectrometry for a new kind of analog produced by polymerization of cryogenically trapped gaseous neutral species. The comparison of these materials emphasizes the importance of ion chemistry processes for the inclusion of nitrogen in molecules constituting Titan's tholins. A statistical approach is also used for the treatment of high resolution mass spectra of these highly complex organic materials. This method allows distinguishing molecular families that can be reconstructed by an ideal copolymer. We investigate several copolymer reconstructions, and we suggest that an HCN (or CH3CN)/C2H4 based copolymer agrees well with the polymeric structure of tholins produced with 5% of methane in nitrogen.
•We analyze different Titan's tholins with orbitrap mass spectrometry.•Results show the importance of ionic chemistry for nitrogen incorporation in tholins.•A statistical approach is used to deal with the high complexity of the mass spectra.•Tholins structures present different molecular families.•Copolymer reconstruction suggests HCN/C2H4 as a possible pattern for polymerization.</description><subject>Aerosols</subject><subject>Analogs</subject><subject>Astrophysics</subject><subject>Atmospheric and Oceanic Physics</subject><subject>Copolymers</subject><subject>Earth and Planetary Astrophysics</subject><subject>High resolution</subject><subject>high resolution mass spectrometry</subject><subject>Mass spectrometry</subject><subject>Methane</subject><subject>nitrogen</subject><subject>Physics</subject><subject>Saturn satellites</subject><subject>Sciences of the Universe</subject><subject>tholins</subject><subject>Titan</subject><subject>Titan's atmosphere</subject><issn>0012-821X</issn><issn>1385-013X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNqNkUFv1DAQhS0EEkvpH-DkG3BImHESe1fiUlVAkVb00kq9WY49u_EqGwc7W2lv3Dn2H_aX4LCICxLqxZafvnl6nsfYG4QSAeWHXUlj6ksBWJegSkB8xhZYLZsCsLp7zhYAKIqlwLuX7FVKOwCQjVwt2M9vfophSwP3gw1xDNFMPswvfuMnM7xNfOpC74eUpQ3FSI63R975bccjpdAffuMhttnHjHxvUuJpJJtd9zTFIzeD41uTuO2yYqawzVh3fPzx8A_6mr3YmD7R-Z_7jN1-_nRzeVWsr798vbxYF6apqqlAqpWsnDWrfLYCWyvRgWrlCq3Z2NYo6YQlVTkhqKqskzL_VeKydkqhw-qMvT_5dqbXY_R7E486GK-vLtZ61gChkShW9zP77sSOMXw_UJr03idLfW8GCoekUTZY4xIVPAGthUQpQWRUnFAbQ0qRNn9jIOi5UL3Tc6F6LlSDyonmKB9PQ5R3c-8p6mQ9DZacj3mJ2gX_v_Ff4AKt0g</recordid><startdate>20141015</startdate><enddate>20141015</enddate><creator>Gautier, Thomas</creator><creator>Carrasco, Nathalie</creator><creator>Schmitz-Afonso, Isabelle</creator><creator>Touboul, David</creator><creator>Szopa, Cyril</creator><creator>Buch, Arnaud</creator><creator>Pernot, Pascal</creator><general>Elsevier B.V</general><general>Elsevier</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7TG</scope><scope>KL.</scope><scope>8FD</scope><scope>H8D</scope><scope>L7M</scope><scope>1XC</scope><scope>VOOES</scope><orcidid>https://orcid.org/0000-0002-0090-4056</orcidid><orcidid>https://orcid.org/0000-0002-0596-6336</orcidid><orcidid>https://orcid.org/0000-0002-9794-5056</orcidid><orcidid>https://orcid.org/0000-0002-2097-7252</orcidid><orcidid>https://orcid.org/0000-0003-2751-774X</orcidid><orcidid>https://orcid.org/0000-0001-8586-6222</orcidid><orcidid>https://orcid.org/0000-0003-0665-0074</orcidid></search><sort><creationdate>20141015</creationdate><title>Nitrogen incorporation in Titan's tholins inferred by high resolution orbitrap mass spectrometry and gas chromatography–mass spectrometry</title><author>Gautier, Thomas ; Carrasco, Nathalie ; Schmitz-Afonso, Isabelle ; Touboul, David ; Szopa, Cyril ; Buch, Arnaud ; Pernot, Pascal</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a533t-1e4763dca963db21bc61d07b691cafcba76d2ce73d22e33cd666566184d771d13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Aerosols</topic><topic>Analogs</topic><topic>Astrophysics</topic><topic>Atmospheric and Oceanic Physics</topic><topic>Copolymers</topic><topic>Earth and Planetary Astrophysics</topic><topic>High resolution</topic><topic>high resolution mass spectrometry</topic><topic>Mass spectrometry</topic><topic>Methane</topic><topic>nitrogen</topic><topic>Physics</topic><topic>Saturn satellites</topic><topic>Sciences of the Universe</topic><topic>tholins</topic><topic>Titan</topic><topic>Titan's atmosphere</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gautier, Thomas</creatorcontrib><creatorcontrib>Carrasco, Nathalie</creatorcontrib><creatorcontrib>Schmitz-Afonso, Isabelle</creatorcontrib><creatorcontrib>Touboul, David</creatorcontrib><creatorcontrib>Szopa, Cyril</creatorcontrib><creatorcontrib>Buch, Arnaud</creatorcontrib><creatorcontrib>Pernot, Pascal</creatorcontrib><collection>CrossRef</collection><collection>Meteorological & Geoastrophysical Abstracts</collection><collection>Meteorological & Geoastrophysical Abstracts - Academic</collection><collection>Technology Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Hyper Article en Ligne (HAL)</collection><collection>Hyper Article en Ligne (HAL) (Open Access)</collection><jtitle>Earth and planetary science letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gautier, Thomas</au><au>Carrasco, Nathalie</au><au>Schmitz-Afonso, Isabelle</au><au>Touboul, David</au><au>Szopa, Cyril</au><au>Buch, Arnaud</au><au>Pernot, Pascal</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Nitrogen incorporation in Titan's tholins inferred by high resolution orbitrap mass spectrometry and gas chromatography–mass spectrometry</atitle><jtitle>Earth and planetary science letters</jtitle><date>2014-10-15</date><risdate>2014</risdate><volume>404</volume><spage>33</spage><epage>42</epage><pages>33-42</pages><issn>0012-821X</issn><eissn>1385-013X</eissn><abstract>Influx of solar photons and heavy charged particles from Saturn's magnetosphere on Titan's atmosphere – mainly comprised of methane and nitrogen – induce an intense organic photochemistry which leads to the formation of a large amount of aerosols in suspension in the atmosphere. In order to infer the role of nitrogen in aerosol formation processes we produced laboratory analogs of Titan's aerosols. In this work, we compare the composition of different analogs by using high resolution mass spectrometry and propose an additional study using gas-chromatography coupled to mass-spectrometry for a new kind of analog produced by polymerization of cryogenically trapped gaseous neutral species. The comparison of these materials emphasizes the importance of ion chemistry processes for the inclusion of nitrogen in molecules constituting Titan's tholins. A statistical approach is also used for the treatment of high resolution mass spectra of these highly complex organic materials. This method allows distinguishing molecular families that can be reconstructed by an ideal copolymer. We investigate several copolymer reconstructions, and we suggest that an HCN (or CH3CN)/C2H4 based copolymer agrees well with the polymeric structure of tholins produced with 5% of methane in nitrogen.
•We analyze different Titan's tholins with orbitrap mass spectrometry.•Results show the importance of ionic chemistry for nitrogen incorporation in tholins.•A statistical approach is used to deal with the high complexity of the mass spectra.•Tholins structures present different molecular families.•Copolymer reconstruction suggests HCN/C2H4 as a possible pattern for polymerization.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.epsl.2014.07.011</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-0090-4056</orcidid><orcidid>https://orcid.org/0000-0002-0596-6336</orcidid><orcidid>https://orcid.org/0000-0002-9794-5056</orcidid><orcidid>https://orcid.org/0000-0002-2097-7252</orcidid><orcidid>https://orcid.org/0000-0003-2751-774X</orcidid><orcidid>https://orcid.org/0000-0001-8586-6222</orcidid><orcidid>https://orcid.org/0000-0003-0665-0074</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Aerosols Analogs Astrophysics Atmospheric and Oceanic Physics Copolymers Earth and Planetary Astrophysics High resolution high resolution mass spectrometry Mass spectrometry Methane nitrogen Physics Saturn satellites Sciences of the Universe tholins Titan Titan's atmosphere |
title | Nitrogen incorporation in Titan's tholins inferred by high resolution orbitrap mass spectrometry and gas chromatography–mass spectrometry |
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