Photochemistry and electron-transfer mechanism of transition metal oxalato complexes excited in the charge transfer band
The photoredox reaction of trisoxalato cobaltate (III) has been studied by means of ultrafast extended x-ray absorption fine structure and optical transient spectroscopy after excitation in the charge-transfer band with 267-nm femtosecond pulses. The Co-O transient bond length changes and the optica...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2008-10, Vol.105 (40), p.15235-15240 |
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| container_title | Proceedings of the National Academy of Sciences - PNAS |
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| creator | Chen, Jie Zhang, Hua Tomov, Ivan V Ding, Xunliang Rentzepis, Peter M |
| description | The photoredox reaction of trisoxalato cobaltate (III) has been studied by means of ultrafast extended x-ray absorption fine structure and optical transient spectroscopy after excitation in the charge-transfer band with 267-nm femtosecond pulses. The Co-O transient bond length changes and the optical spectra and kinetics have been measured and compared with those of ferrioxalate. Data presented here strongly suggest that both of these metal oxalato complexes operate under similar photoredox reaction mechanisms where the primary reaction involves the dissociation of a metal-oxygen bond. These results also indicate that excitation in the charge-transfer band is not a sufficient condition for the intramolecular electron transfer to be the dominant photochemistry reaction mechanism. |
| doi_str_mv | 10.1073/pnas.0806990105 |
| format | Article |
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The Co-O transient bond length changes and the optical spectra and kinetics have been measured and compared with those of ferrioxalate. Data presented here strongly suggest that both of these metal oxalato complexes operate under similar photoredox reaction mechanisms where the primary reaction involves the dissociation of a metal-oxygen bond. These results also indicate that excitation in the charge-transfer band is not a sufficient condition for the intramolecular electron transfer to be the dominant photochemistry reaction mechanism.</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.0806990105</identifier><identifier>PMID: 18832175</identifier><language>eng</language><publisher>United States: National Academy of Sciences</publisher><subject>Absorption spectra ; Charge transfer ; Chemical bonding ; Chemical reactions ; Electron transfer ; Electrons ; Kinetics ; Metals ; Molecules ; Organometallic Compounds - chemistry ; Oxalates ; Oxalates - chemistry ; Photocatalysis ; Photochemistry ; Photolysis ; Physical Sciences ; Sorption ; Transition Elements - chemistry ; X-rays</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2008-10, Vol.105 (40), p.15235-15240</ispartof><rights>Copyright 2008 The National Academy of Sciences of the United States of America</rights><rights>Copyright National Academy of Sciences Oct 7, 2008</rights><rights>2008 by The National Academy of Sciences of the USA</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c523t-1e2fc9fde2b6f011619969c22b9f25d72e95f0f6be3aad2068ded98414b4a88a3</citedby><cites>FETCH-LOGICAL-c523t-1e2fc9fde2b6f011619969c22b9f25d72e95f0f6be3aad2068ded98414b4a88a3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Uhttp://www.pnas.org/content/105/40.cover.gif</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/25464395$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/25464395$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>230,314,723,776,780,799,881,27901,27902,53766,53768,57992,58225</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/18832175$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Chen, Jie</creatorcontrib><creatorcontrib>Zhang, Hua</creatorcontrib><creatorcontrib>Tomov, Ivan V</creatorcontrib><creatorcontrib>Ding, Xunliang</creatorcontrib><creatorcontrib>Rentzepis, Peter M</creatorcontrib><title>Photochemistry and electron-transfer mechanism of transition metal oxalato complexes excited in the charge transfer band</title><title>Proceedings of the National Academy of Sciences - PNAS</title><addtitle>Proc Natl Acad Sci U S A</addtitle><description>The photoredox reaction of trisoxalato cobaltate (III) has been studied by means of ultrafast extended x-ray absorption fine structure and optical transient spectroscopy after excitation in the charge-transfer band with 267-nm femtosecond pulses. The Co-O transient bond length changes and the optical spectra and kinetics have been measured and compared with those of ferrioxalate. Data presented here strongly suggest that both of these metal oxalato complexes operate under similar photoredox reaction mechanisms where the primary reaction involves the dissociation of a metal-oxygen bond. These results also indicate that excitation in the charge-transfer band is not a sufficient condition for the intramolecular electron transfer to be the dominant photochemistry reaction mechanism.</description><subject>Absorption spectra</subject><subject>Charge transfer</subject><subject>Chemical bonding</subject><subject>Chemical reactions</subject><subject>Electron transfer</subject><subject>Electrons</subject><subject>Kinetics</subject><subject>Metals</subject><subject>Molecules</subject><subject>Organometallic Compounds - chemistry</subject><subject>Oxalates</subject><subject>Oxalates - chemistry</subject><subject>Photocatalysis</subject><subject>Photochemistry</subject><subject>Photolysis</subject><subject>Physical Sciences</subject><subject>Sorption</subject><subject>Transition Elements - chemistry</subject><subject>X-rays</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2008</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFkUFvEzEQhVcIREPhzAmwOFTisK3ttR37UglVFJAqgQQ9W17vONlo1w62F6X_Hi-JEuDCydLMN8_z5lXVS4IvCV42V1tv0iWWWCiFCeaPqgXBitSCKfy4WmBMl7VklJ1Vz1LaYIwVl_hpdUakbChZ8kW1-7oOOdg1jH3K8QEZ3yEYwOYYfJ2j8clBRCPYtfF9GlFw6He1z33wpZ7NgMLODCYHZMO4HWAHCcHO9hk61HuU14DKcFwBOsq15Zfn1RNnhgQvDu95dX_74fvNp_ruy8fPN-_vastpk2sC1FnlOqCtcJgQQZQSylLaKkd5t6SguMNOtNAY01EsZAedkoywlhkpTXNeXe91t1M7QmfBlzUGvY39aOKDDqbXf3d8v9ar8FNTLhpCcBG4OAjE8GOClHU5lYVhMB7ClLRQgjFJeAHf_gNuwhR9MacpJk0jCZ2hqz1kY0gpgjtuQrCeI9VzpPoUaZl4_aeBE3_IsADoAMyTJzmuWZEsV5yRd_9BtJuGIcMuF_bVnt2kHOIRppwJ1qhZ682-70zQZhX7pO-_zQYx4WzJJWl-AfoTy-c</recordid><startdate>20081007</startdate><enddate>20081007</enddate><creator>Chen, Jie</creator><creator>Zhang, Hua</creator><creator>Tomov, Ivan V</creator><creator>Ding, Xunliang</creator><creator>Rentzepis, Peter M</creator><general>National Academy of Sciences</general><general>National Acad Sciences</general><scope>FBQ</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>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QR</scope><scope>7SN</scope><scope>7SS</scope><scope>7T5</scope><scope>7TK</scope><scope>7TM</scope><scope>7TO</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>7X8</scope><scope>5PM</scope></search><sort><creationdate>20081007</creationdate><title>Photochemistry and electron-transfer mechanism of transition metal oxalato complexes excited in the charge transfer band</title><author>Chen, Jie ; Zhang, Hua ; Tomov, Ivan V ; Ding, Xunliang ; Rentzepis, Peter M</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c523t-1e2fc9fde2b6f011619969c22b9f25d72e95f0f6be3aad2068ded98414b4a88a3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2008</creationdate><topic>Absorption spectra</topic><topic>Charge transfer</topic><topic>Chemical bonding</topic><topic>Chemical reactions</topic><topic>Electron transfer</topic><topic>Electrons</topic><topic>Kinetics</topic><topic>Metals</topic><topic>Molecules</topic><topic>Organometallic Compounds - chemistry</topic><topic>Oxalates</topic><topic>Oxalates - chemistry</topic><topic>Photocatalysis</topic><topic>Photochemistry</topic><topic>Photolysis</topic><topic>Physical Sciences</topic><topic>Sorption</topic><topic>Transition Elements - chemistry</topic><topic>X-rays</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Jie</creatorcontrib><creatorcontrib>Zhang, Hua</creatorcontrib><creatorcontrib>Tomov, Ivan V</creatorcontrib><creatorcontrib>Ding, Xunliang</creatorcontrib><creatorcontrib>Rentzepis, Peter M</creatorcontrib><collection>AGRIS</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Animal Behavior Abstracts</collection><collection>Bacteriology Abstracts (Microbiology B)</collection><collection>Calcium & Calcified Tissue Abstracts</collection><collection>Chemoreception Abstracts</collection><collection>Ecology Abstracts</collection><collection>Entomology Abstracts (Full archive)</collection><collection>Immunology Abstracts</collection><collection>Neurosciences Abstracts</collection><collection>Nucleic Acids Abstracts</collection><collection>Oncogenes and Growth Factors Abstracts</collection><collection>Virology and AIDS Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>AIDS and Cancer Research Abstracts</collection><collection>Algology Mycology and Protozoology Abstracts (Microbiology C)</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Genetics Abstracts</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Jie</au><au>Zhang, Hua</au><au>Tomov, Ivan V</au><au>Ding, Xunliang</au><au>Rentzepis, Peter M</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Photochemistry and electron-transfer mechanism of transition metal oxalato complexes excited in the charge transfer band</atitle><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle><addtitle>Proc Natl Acad Sci U S A</addtitle><date>2008-10-07</date><risdate>2008</risdate><volume>105</volume><issue>40</issue><spage>15235</spage><epage>15240</epage><pages>15235-15240</pages><issn>0027-8424</issn><eissn>1091-6490</eissn><abstract>The photoredox reaction of trisoxalato cobaltate (III) has been studied by means of ultrafast extended x-ray absorption fine structure and optical transient spectroscopy after excitation in the charge-transfer band with 267-nm femtosecond pulses. The Co-O transient bond length changes and the optical spectra and kinetics have been measured and compared with those of ferrioxalate. Data presented here strongly suggest that both of these metal oxalato complexes operate under similar photoredox reaction mechanisms where the primary reaction involves the dissociation of a metal-oxygen bond. These results also indicate that excitation in the charge-transfer band is not a sufficient condition for the intramolecular electron transfer to be the dominant photochemistry reaction mechanism.</abstract><cop>United States</cop><pub>National Academy of Sciences</pub><pmid>18832175</pmid><doi>10.1073/pnas.0806990105</doi><tpages>6</tpages><oa>free_for_read</oa></addata></record> |
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| subjects | Absorption spectra Charge transfer Chemical bonding Chemical reactions Electron transfer Electrons Kinetics Metals Molecules Organometallic Compounds - chemistry Oxalates Oxalates - chemistry Photocatalysis Photochemistry Photolysis Physical Sciences Sorption Transition Elements - chemistry X-rays |
| title | Photochemistry and electron-transfer mechanism of transition metal oxalato complexes excited in the charge transfer band |
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