Multiphoton dissociation dynamics of BrCl and the BrCl+ cation
Ion imaging methods have enabled identification of three mechanisms by which (79)Br(+) and (35)Cl(+) fragment ions are formed following one-color multiphoton excitation of BrCl molecules in the wavelength range 324.6 > lambda > 311.7 nm. Two-photon excitation within this range populates select...
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| Veröffentlicht in: | Physical chemistry chemical physics : PCCP 2007-01, Vol.9 (41), p.5531-5541 |
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| container_title | Physical chemistry chemical physics : PCCP |
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| creator | VIEUXMAIRE, Olivier P. J HENDRIK NAHLER, N DIXON, Richard N ASHFOLD, Michael N. R |
| description | Ion imaging methods have enabled identification of three mechanisms by which (79)Br(+) and (35)Cl(+) fragment ions are formed following one-color multiphoton excitation of BrCl molecules in the wavelength range 324.6 > lambda > 311.7 nm. Two-photon excitation within this range populates selected vibrational levels (v'= 0-5) of the [X (2)Pi(1/2)]5ssigma Rydberg state. Absorption of a third photon results in branching between (i) photoionization (i.e. removal of the Rydberg electron-a traditional 2 + 1 REMPI process) and (ii)pi* |
| doi_str_mv | 10.1039/b709222a |
| format | Article |
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J ; HENDRIK NAHLER, N ; DIXON, Richard N ; ASHFOLD, Michael N. R</creator><creatorcontrib>VIEUXMAIRE, Olivier P. J ; HENDRIK NAHLER, N ; DIXON, Richard N ; ASHFOLD, Michael N. R</creatorcontrib><description>Ion imaging methods have enabled identification of three mechanisms by which (79)Br(+) and (35)Cl(+) fragment ions are formed following one-color multiphoton excitation of BrCl molecules in the wavelength range 324.6 > lambda > 311.7 nm. Two-photon excitation within this range populates selected vibrational levels (v'= 0-5) of the [X (2)Pi(1/2)]5ssigma Rydberg state. Absorption of a third photon results in branching between (i) photoionization (i.e. removal of the Rydberg electron-a traditional 2 + 1 REMPI process) and (ii)pi*<--pi excitation within the core, resulting in formation of one or more super-excited states with Omega= 1 and configuration [A (2)Pi(1/2)]5ssigma. The fate of the latter states involves a further branching. They can autoionize (yielding BrCl(+)(X (2)Pi) ions in a wider range of v(+) states than formed by direct 2 + 1 REMPI). Further, one-photon absorption by the parent ions resulting from direct ionization or autoionization leads to formation of Br(+) and (energy permitting) Cl(+) fragment ions. Alternatively, the super-excited molecules can fragment to neutral atoms, one of which is in a Rydberg state. Complementary ab initio calculations lead to the conclusion that the observed [Cl**[(3)P(J)]4s + Br/Br*] products result from direct dissociation of the photo-prepared super-excited states, whereas [Br**[(3)P(J)]5p + Cl/Cl*] product formation involves interaction between the [A (2)Pi(1/2)]5ssigma and [X (2)Pi(1/2)]5psigma Rydberg potentials at extended Br-Cl bond lengths. Absorption of one further photon by the resulting Br** and Cl** Rydberg atoms leads to their ionization, and thus their appearance in the Br(+) and Cl(+) fragment ion images.</description><identifier>ISSN: 1463-9076</identifier><identifier>EISSN: 1463-9084</identifier><identifier>DOI: 10.1039/b709222a</identifier><identifier>PMID: 17957309</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Algorithms ; Bromides - chemistry ; Cations ; Chemistry ; Chlorides - chemistry ; Energy Transfer - radiation effects ; Exact sciences and technology ; General and physical chemistry ; Kinetics ; Models, Chemical ; Photolysis - radiation effects ; Photons ; Radiation, Ionizing ; Spectrum Analysis - methods ; Ultraviolet Rays</subject><ispartof>Physical chemistry chemical physics : PCCP, 2007-01, Vol.9 (41), p.5531-5541</ispartof><rights>2007 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c331t-39a434c13e3a0ef4eac83a97d46758fa952ce990c7aef6f6b67027f475eafab43</citedby><cites>FETCH-LOGICAL-c331t-39a434c13e3a0ef4eac83a97d46758fa952ce990c7aef6f6b67027f475eafab43</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,2831,27924,27925</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=19202889$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/17957309$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>VIEUXMAIRE, Olivier P. J</creatorcontrib><creatorcontrib>HENDRIK NAHLER, N</creatorcontrib><creatorcontrib>DIXON, Richard N</creatorcontrib><creatorcontrib>ASHFOLD, Michael N. R</creatorcontrib><title>Multiphoton dissociation dynamics of BrCl and the BrCl+ cation</title><title>Physical chemistry chemical physics : PCCP</title><addtitle>Phys Chem Chem Phys</addtitle><description>Ion imaging methods have enabled identification of three mechanisms by which (79)Br(+) and (35)Cl(+) fragment ions are formed following one-color multiphoton excitation of BrCl molecules in the wavelength range 324.6 > lambda > 311.7 nm. Two-photon excitation within this range populates selected vibrational levels (v'= 0-5) of the [X (2)Pi(1/2)]5ssigma Rydberg state. Absorption of a third photon results in branching between (i) photoionization (i.e. removal of the Rydberg electron-a traditional 2 + 1 REMPI process) and (ii)pi*<--pi excitation within the core, resulting in formation of one or more super-excited states with Omega= 1 and configuration [A (2)Pi(1/2)]5ssigma. The fate of the latter states involves a further branching. They can autoionize (yielding BrCl(+)(X (2)Pi) ions in a wider range of v(+) states than formed by direct 2 + 1 REMPI). Further, one-photon absorption by the parent ions resulting from direct ionization or autoionization leads to formation of Br(+) and (energy permitting) Cl(+) fragment ions. Alternatively, the super-excited molecules can fragment to neutral atoms, one of which is in a Rydberg state. Complementary ab initio calculations lead to the conclusion that the observed [Cl**[(3)P(J)]4s + Br/Br*] products result from direct dissociation of the photo-prepared super-excited states, whereas [Br**[(3)P(J)]5p + Cl/Cl*] product formation involves interaction between the [A (2)Pi(1/2)]5ssigma and [X (2)Pi(1/2)]5psigma Rydberg potentials at extended Br-Cl bond lengths. Absorption of one further photon by the resulting Br** and Cl** Rydberg atoms leads to their ionization, and thus their appearance in the Br(+) and Cl(+) fragment ion images.</description><subject>Algorithms</subject><subject>Bromides - chemistry</subject><subject>Cations</subject><subject>Chemistry</subject><subject>Chlorides - chemistry</subject><subject>Energy Transfer - radiation effects</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Kinetics</subject><subject>Models, Chemical</subject><subject>Photolysis - radiation effects</subject><subject>Photons</subject><subject>Radiation, Ionizing</subject><subject>Spectrum Analysis - methods</subject><subject>Ultraviolet Rays</subject><issn>1463-9076</issn><issn>1463-9084</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2007</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpF0M1LwzAYBvAgiptT8C-QXhRBqvlq0lwEHX7BxIuey9s0YZG2mUl72H9vt1V3et8HfjyHB6Fzgm8JZuqulFhRSuEATQkXLFU454f_vxQTdBLjN8aYZIQdowmRKpMMqym6f-_rzq2WvvNtUrkYvXbQuU1Yt9A4HRNvk8cwrxNoq6Rbmm24SfRWnaIjC3U0Z-Odoa_np8_5a7r4eHmbPyxSzRjpUqaAM64JMwywsdyAzhkoWXEhs9yCyqg2SmEtwVhhRSkkptJymRmwUHI2Q1e73lXwP72JXdG4qE1dQ2t8HwuRcyqloAO83kEdfIzB2GIVXANhXRBcbLYq_rYa6MXY2ZeNqfZwHGcAlyOAqKG2AVrt4t4pimmeK_YLG4BwEA</recordid><startdate>20070101</startdate><enddate>20070101</enddate><creator>VIEUXMAIRE, Olivier P. J</creator><creator>HENDRIK NAHLER, N</creator><creator>DIXON, Richard N</creator><creator>ASHFOLD, Michael N. R</creator><general>Royal Society of Chemistry</general><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20070101</creationdate><title>Multiphoton dissociation dynamics of BrCl and the BrCl+ cation</title><author>VIEUXMAIRE, Olivier P. J ; HENDRIK NAHLER, N ; DIXON, Richard N ; ASHFOLD, Michael N. R</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c331t-39a434c13e3a0ef4eac83a97d46758fa952ce990c7aef6f6b67027f475eafab43</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2007</creationdate><topic>Algorithms</topic><topic>Bromides - chemistry</topic><topic>Cations</topic><topic>Chemistry</topic><topic>Chlorides - chemistry</topic><topic>Energy Transfer - radiation effects</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Kinetics</topic><topic>Models, Chemical</topic><topic>Photolysis - radiation effects</topic><topic>Photons</topic><topic>Radiation, Ionizing</topic><topic>Spectrum Analysis - methods</topic><topic>Ultraviolet Rays</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>VIEUXMAIRE, Olivier P. J</creatorcontrib><creatorcontrib>HENDRIK NAHLER, N</creatorcontrib><creatorcontrib>DIXON, Richard N</creatorcontrib><creatorcontrib>ASHFOLD, Michael N. R</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Physical chemistry chemical physics : PCCP</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>VIEUXMAIRE, Olivier P. J</au><au>HENDRIK NAHLER, N</au><au>DIXON, Richard N</au><au>ASHFOLD, Michael N. R</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Multiphoton dissociation dynamics of BrCl and the BrCl+ cation</atitle><jtitle>Physical chemistry chemical physics : PCCP</jtitle><addtitle>Phys Chem Chem Phys</addtitle><date>2007-01-01</date><risdate>2007</risdate><volume>9</volume><issue>41</issue><spage>5531</spage><epage>5541</epage><pages>5531-5541</pages><issn>1463-9076</issn><eissn>1463-9084</eissn><abstract>Ion imaging methods have enabled identification of three mechanisms by which (79)Br(+) and (35)Cl(+) fragment ions are formed following one-color multiphoton excitation of BrCl molecules in the wavelength range 324.6 > lambda > 311.7 nm. Two-photon excitation within this range populates selected vibrational levels (v'= 0-5) of the [X (2)Pi(1/2)]5ssigma Rydberg state. Absorption of a third photon results in branching between (i) photoionization (i.e. removal of the Rydberg electron-a traditional 2 + 1 REMPI process) and (ii)pi*<--pi excitation within the core, resulting in formation of one or more super-excited states with Omega= 1 and configuration [A (2)Pi(1/2)]5ssigma. The fate of the latter states involves a further branching. They can autoionize (yielding BrCl(+)(X (2)Pi) ions in a wider range of v(+) states than formed by direct 2 + 1 REMPI). Further, one-photon absorption by the parent ions resulting from direct ionization or autoionization leads to formation of Br(+) and (energy permitting) Cl(+) fragment ions. Alternatively, the super-excited molecules can fragment to neutral atoms, one of which is in a Rydberg state. Complementary ab initio calculations lead to the conclusion that the observed [Cl**[(3)P(J)]4s + Br/Br*] products result from direct dissociation of the photo-prepared super-excited states, whereas [Br**[(3)P(J)]5p + Cl/Cl*] product formation involves interaction between the [A (2)Pi(1/2)]5ssigma and [X (2)Pi(1/2)]5psigma Rydberg potentials at extended Br-Cl bond lengths. Absorption of one further photon by the resulting Br** and Cl** Rydberg atoms leads to their ionization, and thus their appearance in the Br(+) and Cl(+) fragment ion images.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><pmid>17957309</pmid><doi>10.1039/b709222a</doi><tpages>11</tpages></addata></record> |
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| source | MEDLINE; Royal Society of Chemistry Journals Archive (1841-2007); Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
| subjects | Algorithms Bromides - chemistry Cations Chemistry Chlorides - chemistry Energy Transfer - radiation effects Exact sciences and technology General and physical chemistry Kinetics Models, Chemical Photolysis - radiation effects Photons Radiation, Ionizing Spectrum Analysis - methods Ultraviolet Rays |
| title | Multiphoton dissociation dynamics of BrCl and the BrCl+ cation |
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