A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations
DCl(+)(X (2)Pi(32),v(+")=0) cations have been prepared by 2+1 resonance enhanced multiphoton ionization, and their subsequent fragmentation following excitation at numerous wavelengths in the range of 240-350 nm studied by velocity map imaging of the resulting Cl(+) products. This range of exci...
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| Veröffentlicht in: | The Journal of chemical physics 2006-11, Vol.125 (20), p.204312-204312 |
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| container_title | The Journal of chemical physics |
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| creator | Webb, Alexander D Nahler, N Hendrik Dixon, Richard N Ashfold, Michael N R |
| description | DCl(+)(X (2)Pi(32),v(+")=0) cations have been prepared by 2+1 resonance enhanced multiphoton ionization, and their subsequent fragmentation following excitation at numerous wavelengths in the range of 240-350 nm studied by velocity map imaging of the resulting Cl(+) products. This range of excitation wavelengths allows selective population of A (2)Sigma(+) state levels with all vibrational (v(+')) quantum numbers in the range 0< or =v(+')< or =15. Image analysis yields wavelength dependent branching ratios and recoil anisotropies of the various D+Cl(+) ((3)P(J), (1)D, and (1)S) product channels. Levels with 10< or =v(+')< or =15 have sufficient energy to predissociate, forming D+Cl(+)((3)P(J)) products with perpendicular recoil anisotropies-consistent with the A (2)Sigma(+) |
| doi_str_mv | 10.1063/1.2390714 |
| format | Article |
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This range of excitation wavelengths allows selective population of A (2)Sigma(+) state levels with all vibrational (v(+')) quantum numbers in the range 0< or =v(+')< or =15. Image analysis yields wavelength dependent branching ratios and recoil anisotropies of the various D+Cl(+) ((3)P(J), (1)D, and (1)S) product channels. Levels with 10< or =v(+')< or =15 have sufficient energy to predissociate, forming D+Cl(+)((3)P(J)) products with perpendicular recoil anisotropies-consistent with the A (2)Sigma(+)<--X (2)Pi parent excitation and subsequent fragmentation on a time scale that is fast compared with the parent rotational period. Branching into the various spin-orbit states of the Cl(+)((3)P(J)) product is found to depend sensitively upon v(+') and, in the case of the v(+')=13 level, to vary with the precise choice of excitation wavelength within the A (2)Sigma(+)<--X (2)Pi(13,0) band. Such variations have been rationalized qualitatively in terms of the differing contributions made to the overall predissociation rate of DCl(+)(A,v(+')) molecules by coupling to repulsive states of (4)Pi, (4)Sigma(-), and (2)Sigma(-) symmetries, all of which are calculated to cross the outer limb of the A (2)Sigma(+) state potential at energies close to that of the v(+')=10 level. Cl(+)((3)P(J)) fragments are detected weakly following excitation to A (2)Sigma(+) state levels with v(+')=0 or 1, Cl(+)((1)D) fragments dominate the ion yield when exciting via 2< or =v(+')< or =6 and via v(+')=9, while Cl(+)((1)S) fragments dominate the Cl(+) images obtained when exciting via levels with v(+')=7 and 8. Analysis of wavelength resolved action spectra for forming these Cl(+) ions and of the resulting Cl(+) ion images shows that (i) these ions all arise via two photon absorption processes, resonance enhanced at the one photon energy by the various A(v(+')<10) levels, (ii) the first A (2)Sigma(+)<--X (2)Pi absorption step is saturated under the conditions required to observe significant two photon dissociation, and (iii) the final absorption step from the resonance enhancing A(v(+')) level involves a parallel transition.]]></description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/1.2390714</identifier><identifier>PMID: 17144705</identifier><language>eng</language><publisher>United States</publisher><ispartof>The Journal of chemical physics, 2006-11, Vol.125 (20), p.204312-204312</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c213t-b239b8e192e891490086bfe9c52d1f929639d22093af1b2123962d9e6fa9710c3</citedby><cites>FETCH-LOGICAL-c213t-b239b8e192e891490086bfe9c52d1f929639d22093af1b2123962d9e6fa9710c3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/17144705$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Webb, Alexander D</creatorcontrib><creatorcontrib>Nahler, N Hendrik</creatorcontrib><creatorcontrib>Dixon, Richard N</creatorcontrib><creatorcontrib>Ashfold, Michael N R</creatorcontrib><title>A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations</title><title>The Journal of chemical physics</title><addtitle>J Chem Phys</addtitle><description><![CDATA[DCl(+)(X (2)Pi(32),v(+")=0) cations have been prepared by 2+1 resonance enhanced multiphoton ionization, and their subsequent fragmentation following excitation at numerous wavelengths in the range of 240-350 nm studied by velocity map imaging of the resulting Cl(+) products. This range of excitation wavelengths allows selective population of A (2)Sigma(+) state levels with all vibrational (v(+')) quantum numbers in the range 0< or =v(+')< or =15. Image analysis yields wavelength dependent branching ratios and recoil anisotropies of the various D+Cl(+) ((3)P(J), (1)D, and (1)S) product channels. Levels with 10< or =v(+')< or =15 have sufficient energy to predissociate, forming D+Cl(+)((3)P(J)) products with perpendicular recoil anisotropies-consistent with the A (2)Sigma(+)<--X (2)Pi parent excitation and subsequent fragmentation on a time scale that is fast compared with the parent rotational period. Branching into the various spin-orbit states of the Cl(+)((3)P(J)) product is found to depend sensitively upon v(+') and, in the case of the v(+')=13 level, to vary with the precise choice of excitation wavelength within the A (2)Sigma(+)<--X (2)Pi(13,0) band. Such variations have been rationalized qualitatively in terms of the differing contributions made to the overall predissociation rate of DCl(+)(A,v(+')) molecules by coupling to repulsive states of (4)Pi, (4)Sigma(-), and (2)Sigma(-) symmetries, all of which are calculated to cross the outer limb of the A (2)Sigma(+) state potential at energies close to that of the v(+')=10 level. Cl(+)((3)P(J)) fragments are detected weakly following excitation to A (2)Sigma(+) state levels with v(+')=0 or 1, Cl(+)((1)D) fragments dominate the ion yield when exciting via 2< or =v(+')< or =6 and via v(+')=9, while Cl(+)((1)S) fragments dominate the Cl(+) images obtained when exciting via levels with v(+')=7 and 8. Analysis of wavelength resolved action spectra for forming these Cl(+) ions and of the resulting Cl(+) ion images shows that (i) these ions all arise via two photon absorption processes, resonance enhanced at the one photon energy by the various A(v(+')<10) levels, (ii) the first A (2)Sigma(+)<--X (2)Pi absorption step is saturated under the conditions required to observe significant two photon dissociation, and (iii) the final absorption step from the resonance enhancing A(v(+')) level involves a parallel transition.]]></description><issn>0021-9606</issn><issn>1089-7690</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2006</creationdate><recordtype>article</recordtype><recordid>eNpF0E1Lw0AQBuBFFFurB_-A7EkQSZ3ZTTfZY6mfUPCi57DZTNpIkq3ZjdJ_b0oDnuYwz7wwL2PXCHMEJR9wLqSGBOMTNkVIdZQoDadsCiAw0grUhF14_wUAmIj4nE1wsHECiymzS_5DtbNV2PPG7HjVmE3VbrgPfbHnruRhS9y1xE1b8PDr-G7rgmt5UXk_XJlQudYfnA8mUOSpJhuo4I-r-p7b4_qSnZWm9nQ1zhn7fH76WL1G6_eXt9VyHVmBMkT58ESeEmpBqcZYA6QqL0nbhSiw1EIrqQshQEtTYi5w4EoUmlRpdIJg5YzdHnN3nfvuyYesqbylujYtud5nKhWodSoHeHeEtnPed1Rmu254vNtnCNmh0QyzsdHB3oyhfd5Q8S_HCuUfm4ZvSA</recordid><startdate>20061128</startdate><enddate>20061128</enddate><creator>Webb, Alexander D</creator><creator>Nahler, N Hendrik</creator><creator>Dixon, Richard N</creator><creator>Ashfold, Michael N R</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20061128</creationdate><title>A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations</title><author>Webb, Alexander D ; Nahler, N Hendrik ; Dixon, Richard N ; Ashfold, Michael N R</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c213t-b239b8e192e891490086bfe9c52d1f929639d22093af1b2123962d9e6fa9710c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2006</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Webb, Alexander D</creatorcontrib><creatorcontrib>Nahler, N Hendrik</creatorcontrib><creatorcontrib>Dixon, Richard N</creatorcontrib><creatorcontrib>Ashfold, Michael N R</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>The Journal of chemical physics</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Webb, Alexander D</au><au>Nahler, N Hendrik</au><au>Dixon, Richard N</au><au>Ashfold, Michael N R</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations</atitle><jtitle>The Journal of chemical physics</jtitle><addtitle>J Chem Phys</addtitle><date>2006-11-28</date><risdate>2006</risdate><volume>125</volume><issue>20</issue><spage>204312</spage><epage>204312</epage><pages>204312-204312</pages><issn>0021-9606</issn><eissn>1089-7690</eissn><abstract><![CDATA[DCl(+)(X (2)Pi(32),v(+")=0) cations have been prepared by 2+1 resonance enhanced multiphoton ionization, and their subsequent fragmentation following excitation at numerous wavelengths in the range of 240-350 nm studied by velocity map imaging of the resulting Cl(+) products. This range of excitation wavelengths allows selective population of A (2)Sigma(+) state levels with all vibrational (v(+')) quantum numbers in the range 0< or =v(+')< or =15. Image analysis yields wavelength dependent branching ratios and recoil anisotropies of the various D+Cl(+) ((3)P(J), (1)D, and (1)S) product channels. Levels with 10< or =v(+')< or =15 have sufficient energy to predissociate, forming D+Cl(+)((3)P(J)) products with perpendicular recoil anisotropies-consistent with the A (2)Sigma(+)<--X (2)Pi parent excitation and subsequent fragmentation on a time scale that is fast compared with the parent rotational period. Branching into the various spin-orbit states of the Cl(+)((3)P(J)) product is found to depend sensitively upon v(+') and, in the case of the v(+')=13 level, to vary with the precise choice of excitation wavelength within the A (2)Sigma(+)<--X (2)Pi(13,0) band. Such variations have been rationalized qualitatively in terms of the differing contributions made to the overall predissociation rate of DCl(+)(A,v(+')) molecules by coupling to repulsive states of (4)Pi, (4)Sigma(-), and (2)Sigma(-) symmetries, all of which are calculated to cross the outer limb of the A (2)Sigma(+) state potential at energies close to that of the v(+')=10 level. Cl(+)((3)P(J)) fragments are detected weakly following excitation to A (2)Sigma(+) state levels with v(+')=0 or 1, Cl(+)((1)D) fragments dominate the ion yield when exciting via 2< or =v(+')< or =6 and via v(+')=9, while Cl(+)((1)S) fragments dominate the Cl(+) images obtained when exciting via levels with v(+')=7 and 8. Analysis of wavelength resolved action spectra for forming these Cl(+) ions and of the resulting Cl(+) ion images shows that (i) these ions all arise via two photon absorption processes, resonance enhanced at the one photon energy by the various A(v(+')<10) levels, (ii) the first A (2)Sigma(+)<--X (2)Pi absorption step is saturated under the conditions required to observe significant two photon dissociation, and (iii) the final absorption step from the resonance enhancing A(v(+')) level involves a parallel transition.]]></abstract><cop>United States</cop><pmid>17144705</pmid><doi>10.1063/1.2390714</doi><tpages>1</tpages></addata></record> |
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| source | AIP Journals Complete; AIP Digital Archive |
| title | A velocity map imaging study of the one and two photon dissociations of state-selected DCl+ cations |
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