Probing the Threshold to H Atom Transfer along a Hydrogen-Bonded Ammonia Wire
We characterized the entrance channel, reaction threshold, and mechanism of an excited-state H atom transfer reaction along a unidirectionally hydrogenbonded "wire"$-O-H \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot N$. Excitation of supersonically...
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| Veröffentlicht in: | Science (American Association for the Advancement of Science) 2003-12, Vol.302 (5651), p.1736-1739 |
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| creator | Tanner, Christian Manca, Carine Leutwyler, Samuel |
| description | We characterized the entrance channel, reaction threshold, and mechanism of an excited-state H atom transfer reaction along a unidirectionally hydrogenbonded "wire"$-O-H \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot N$. Excitation of supersonically cooled$7-hydroxyquinoline\cdot (NH_3)_3$to its vibrationless S1state produces no reaction, whereas excitation of ammonia-wire vibrations induces H atom transfer with a reaction threshold ≈ 200 wave numbers. Further translocation steps along the wire produce the S1state$7-ketoquinoline\cdot (NH_3)_3$tautomer. Ab initio calculations show that proton and electron movement along the wire are closely coupled. The rate-controlling S1state barriers arise from crossings of a ππ*with a Rydberg-type$\pi\sigma^\ast$state. |
| doi_str_mv | 10.1126/science.1091708 |
| format | Article |
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Excitation of supersonically cooled$7-hydroxyquinoline\cdot (NH_3)_3$to its vibrationless S1state produces no reaction, whereas excitation of ammonia-wire vibrations induces H atom transfer with a reaction threshold ≈ 200 wave numbers. Further translocation steps along the wire produce the S1state$7-ketoquinoline\cdot (NH_3)_3$tautomer. Ab initio calculations show that proton and electron movement along the wire are closely coupled. The rate-controlling S1state barriers arise from crossings of a ππ*with a Rydberg-type$\pi\sigma^\ast$state.</description><identifier>ISSN: 0036-8075</identifier><identifier>EISSN: 1095-9203</identifier><identifier>DOI: 10.1126/science.1091708</identifier><identifier>PMID: 14657491</identifier><identifier>CODEN: SCIEAS</identifier><language>eng</language><publisher>Washington, DC: American Association for the Advancement of Science</publisher><subject>Ammonia ; Atoms ; Atoms & subatomic particles ; Chemistry ; Energy ; Exact sciences and technology ; Exhibits ; Experiments ; Fluorescence ; Hydrogen ; Inhalants ; Ionization ; Lasers ; Lead ; Molecules ; Observations ; Orbitals ; Organic Chemistry ; Properties ; Protons ; Spectral bands ; Spectroscopy ; Tautomers ; Vibration</subject><ispartof>Science (American Association for the Advancement of Science), 2003-12, Vol.302 (5651), p.1736-1739</ispartof><rights>Copyright 2003 American Association for the Advancement of Science</rights><rights>2004 INIST-CNRS</rights><rights>COPYRIGHT 2003 American Association for the Advancement of Science</rights><rights>COPYRIGHT 2003 American Association for the Advancement of Science</rights><rights>Copyright American Association for the Advancement of Science Dec 5, 2003</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c751t-9e9226fef9bfc37c5e50a3dfb886196cb526801d0996cf553fe7c6ed9066e6193</citedby><cites>FETCH-LOGICAL-c751t-9e9226fef9bfc37c5e50a3dfb886196cb526801d0996cf553fe7c6ed9066e6193</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/3835881$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/3835881$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>314,777,781,800,2871,2872,27905,27906,57998,58231</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=15345283$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/14657491$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Tanner, Christian</creatorcontrib><creatorcontrib>Manca, Carine</creatorcontrib><creatorcontrib>Leutwyler, Samuel</creatorcontrib><title>Probing the Threshold to H Atom Transfer along a Hydrogen-Bonded Ammonia Wire</title><title>Science (American Association for the Advancement of Science)</title><addtitle>Science</addtitle><description>We characterized the entrance channel, reaction threshold, and mechanism of an excited-state H atom transfer reaction along a unidirectionally hydrogenbonded "wire"$-O-H \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot N$. Excitation of supersonically cooled$7-hydroxyquinoline\cdot (NH_3)_3$to its vibrationless S1state produces no reaction, whereas excitation of ammonia-wire vibrations induces H atom transfer with a reaction threshold ≈ 200 wave numbers. Further translocation steps along the wire produce the S1state$7-ketoquinoline\cdot (NH_3)_3$tautomer. Ab initio calculations show that proton and electron movement along the wire are closely coupled. The rate-controlling S1state barriers arise from crossings of a ππ*with a Rydberg-type$\pi\sigma^\ast$state.</description><subject>Ammonia</subject><subject>Atoms</subject><subject>Atoms & subatomic particles</subject><subject>Chemistry</subject><subject>Energy</subject><subject>Exact sciences and technology</subject><subject>Exhibits</subject><subject>Experiments</subject><subject>Fluorescence</subject><subject>Hydrogen</subject><subject>Inhalants</subject><subject>Ionization</subject><subject>Lasers</subject><subject>Lead</subject><subject>Molecules</subject><subject>Observations</subject><subject>Orbitals</subject><subject>Organic Chemistry</subject><subject>Properties</subject><subject>Protons</subject><subject>Spectral 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Samuel</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Probing the Threshold to H Atom Transfer along a Hydrogen-Bonded Ammonia Wire</atitle><jtitle>Science (American Association for the Advancement of Science)</jtitle><addtitle>Science</addtitle><date>2003-12-05</date><risdate>2003</risdate><volume>302</volume><issue>5651</issue><spage>1736</spage><epage>1739</epage><pages>1736-1739</pages><issn>0036-8075</issn><eissn>1095-9203</eissn><coden>SCIEAS</coden><abstract>We characterized the entrance channel, reaction threshold, and mechanism of an excited-state H atom transfer reaction along a unidirectionally hydrogenbonded "wire"$-O-H \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot NH_3 \cdot \cdot \cdot N$. Excitation of supersonically cooled$7-hydroxyquinoline\cdot (NH_3)_3$to its vibrationless S1state produces no reaction, whereas excitation of ammonia-wire vibrations induces H atom transfer with a reaction threshold ≈ 200 wave numbers. Further translocation steps along the wire produce the S1state$7-ketoquinoline\cdot (NH_3)_3$tautomer. Ab initio calculations show that proton and electron movement along the wire are closely coupled. The rate-controlling S1state barriers arise from crossings of a ππ*with a Rydberg-type$\pi\sigma^\ast$state.</abstract><cop>Washington, DC</cop><pub>American Association for the Advancement of Science</pub><pmid>14657491</pmid><doi>10.1126/science.1091708</doi><tpages>4</tpages></addata></record> |
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| source | Science Magazine; Jstor Complete Legacy |
| subjects | Ammonia Atoms Atoms & subatomic particles Chemistry Energy Exact sciences and technology Exhibits Experiments Fluorescence Hydrogen Inhalants Ionization Lasers Lead Molecules Observations Orbitals Organic Chemistry Properties Protons Spectral bands Spectroscopy Tautomers Vibration |
| title | Probing the Threshold to H Atom Transfer along a Hydrogen-Bonded Ammonia Wire |
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