Electric field-controlled dissociation and association of porphyrin J-aggregates in aqueous solution.
Identifieur interne : 001E48 ( PubMed/Curation ); précédent : 001E47; suivant : 001E49Electric field-controlled dissociation and association of porphyrin J-aggregates in aqueous solution.
Auteurs : Kazuaki Nakata [Japon] ; Takayoshi Kobayashi ; Eiji TokunagaSource :
- Physical chemistry chemical physics : PCCP [ 1463-9084 ] ; 2011.
Descripteurs français
- KwdFr :
- MESH :
English descriptors
- KwdEn :
- MESH :
- chemical , chemistry : Porphyrins, Water.
- Electromagnetic Fields, Solutions, Spectrophotometry, Ultraviolet.
Abstract
The electrooptic effects of porphyrin J-aggregates of tetraphenyl porphyrin tetrasulfonic acid (TPPS) in aqueous solution were studied using electroabsorption (EA) spectroscopy. When the J-aggregates were three-dimensionally distributed, the EA spectra exhibited broadening in the exciton band. When a DC or AC electric field was applied for a long time, the J-aggregates with KCl were dissociated into monomers via N-mers (N = 2-4) as intermediate states, while those without KCl had an increase in aggregation. The EA spectra showed a red shift in the exciton band for N-mers, which indicates that N-mers are isolated microaggregates with a coherent aggregation number N, and isolated microaggregates have not been microscopically or spectrally observed until now. The estimated third-order nonlinear optical susceptibility χ((3)) for EA spectra in aqueous solution was 10(4) times larger than that in a polymer film. The molecular rearrangement model was applied to a variety of orientational distributions and the results were explained fairly well. The contribution of the electric double layer is the most probable reason for the large enhancement of χ((3)) for the solution sample. The dynamic equilibrium between two types of monomers, J-aggregates of various aggregation numbers and cations such as K(+) and H(+) was investigated to reveal that K(+) is more loosely bound to the constituent monomers in J-aggregates than H(+). Equilibrium equations also show that well-grown aggregates with N > 15 tend to dominate in a solution of J-aggregates, which explains why only well-developed aggregates can be observed spectroscopically.
DOI: 10.1039/c1cp21964b
PubMed: 21909514
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When the J-aggregates were three-dimensionally distributed, the EA spectra exhibited broadening in the exciton band. When a DC or AC electric field was applied for a long time, the J-aggregates with KCl were dissociated into monomers via N-mers (N = 2-4) as intermediate states, while those without KCl had an increase in aggregation. The EA spectra showed a red shift in the exciton band for N-mers, which indicates that N-mers are isolated microaggregates with a coherent aggregation number N, and isolated microaggregates have not been microscopically or spectrally observed until now. The estimated third-order nonlinear optical susceptibility χ((3)) for EA spectra in aqueous solution was 10(4) times larger than that in a polymer film. The molecular rearrangement model was applied to a variety of orientational distributions and the results were explained fairly well. The contribution of the electric double layer is the most probable reason for the large enhancement of χ((3)) for the solution sample. The dynamic equilibrium between two types of monomers, J-aggregates of various aggregation numbers and cations such as K(+) and H(+) was investigated to reveal that K(+) is more loosely bound to the constituent monomers in J-aggregates than H(+). Equilibrium equations also show that well-grown aggregates with N > 15 tend to dominate in a solution of J-aggregates, which explains why only well-developed aggregates can be observed spectroscopically.</div></front></TEI><pubmed><MedlineCitation Status="MEDLINE" Owner="NLM"><PMID Version="1">21909514</PMID><DateCompleted><Year>2012</Year><Month>01</Month><Day>26</Day></DateCompleted><DateRevised><Year>2013</Year><Month>11</Month><Day>21</Day></DateRevised><Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1463-9084</ISSN><JournalIssue CitedMedium="Internet"><Volume>13</Volume><Issue>39</Issue><PubDate><Year>2011</Year><Month>Oct</Month><Day>21</Day></PubDate></JournalIssue><Title>Physical chemistry chemical physics : PCCP</Title><ISOAbbreviation>Phys Chem Chem Phys</ISOAbbreviation></Journal><ArticleTitle>Electric field-controlled dissociation and association of porphyrin J-aggregates in aqueous solution.</ArticleTitle><Pagination><MedlinePgn>17756-67</MedlinePgn></Pagination><ELocationID EIdType="doi" ValidYN="Y">10.1039/c1cp21964b</ELocationID><Abstract><AbstractText>The electrooptic effects of porphyrin J-aggregates of tetraphenyl porphyrin tetrasulfonic acid (TPPS) in aqueous solution were studied using electroabsorption (EA) spectroscopy. When the J-aggregates were three-dimensionally distributed, the EA spectra exhibited broadening in the exciton band. When a DC or AC electric field was applied for a long time, the J-aggregates with KCl were dissociated into monomers via N-mers (N = 2-4) as intermediate states, while those without KCl had an increase in aggregation. The EA spectra showed a red shift in the exciton band for N-mers, which indicates that N-mers are isolated microaggregates with a coherent aggregation number N, and isolated microaggregates have not been microscopically or spectrally observed until now. The estimated third-order nonlinear optical susceptibility χ((3)) for EA spectra in aqueous solution was 10(4) times larger than that in a polymer film. The molecular rearrangement model was applied to a variety of orientational distributions and the results were explained fairly well. The contribution of the electric double layer is the most probable reason for the large enhancement of χ((3)) for the solution sample. The dynamic equilibrium between two types of monomers, J-aggregates of various aggregation numbers and cations such as K(+) and H(+) was investigated to reveal that K(+) is more loosely bound to the constituent monomers in J-aggregates than H(+). Equilibrium equations also show that well-grown aggregates with N > 15 tend to dominate in a solution of J-aggregates, which explains why only well-developed aggregates can be observed spectroscopically.</AbstractText><CopyrightInformation>This journal is © the Owner Societies 2011</CopyrightInformation></Abstract><AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Nakata</LastName><ForeName>Kazuaki</ForeName><Initials>K</Initials><AffiliationInfo><Affiliation>Department of Physics, Faculty of Science, Tokyo University of Science, 1-3 Kagurazaka, Tokyo 162-8601, Japan.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Kobayashi</LastName><ForeName>Takayoshi</ForeName><Initials>T</Initials></Author><Author ValidYN="Y"><LastName>Tokunaga</LastName><ForeName>Eiji</ForeName><Initials>E</Initials></Author></AuthorList><Language>eng</Language><PublicationTypeList><PublicationType UI="D016428">Journal Article</PublicationType><PublicationType UI="D013485">Research Support, Non-U.S. Gov't</PublicationType></PublicationTypeList><ArticleDate DateType="Electronic"><Year>2011</Year><Month>09</Month><Day>09</Day></ArticleDate></Article><MedlineJournalInfo><Country>England</Country><MedlineTA>Phys Chem Chem Phys</MedlineTA><NlmUniqueID>100888160</NlmUniqueID><ISSNLinking>1463-9076</ISSNLinking></MedlineJournalInfo><ChemicalList><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance UI="D011166">Porphyrins</NameOfSubstance></Chemical><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance UI="D012996">Solutions</NameOfSubstance></Chemical><Chemical><RegistryNumber>059QF0KO0R</RegistryNumber><NameOfSubstance UI="D014867">Water</NameOfSubstance></Chemical></ChemicalList><CitationSubset>IM</CitationSubset><MeshHeadingList><MeshHeading><DescriptorName UI="D004574" MajorTopicYN="Y">Electromagnetic Fields</DescriptorName></MeshHeading><MeshHeading><DescriptorName UI="D011166" MajorTopicYN="N">Porphyrins</DescriptorName><QualifierName UI="Q000737" MajorTopicYN="Y">chemistry</QualifierName></MeshHeading><MeshHeading><DescriptorName UI="D012996" MajorTopicYN="N">Solutions</DescriptorName></MeshHeading><MeshHeading><DescriptorName UI="D013056" MajorTopicYN="N">Spectrophotometry, Ultraviolet</DescriptorName></MeshHeading><MeshHeading><DescriptorName UI="D014867" MajorTopicYN="N">Water</DescriptorName><QualifierName UI="Q000737" MajorTopicYN="N">chemistry</QualifierName></MeshHeading></MeshHeadingList></MedlineCitation><PubmedData><History><PubMedPubDate PubStatus="entrez"><Year>2011</Year><Month>9</Month><Day>13</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="pubmed"><Year>2011</Year><Month>9</Month><Day>13</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="medline"><Year>2012</Year><Month>1</Month><Day>27</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate></History><PublicationStatus>ppublish</PublicationStatus><ArticleIdList><ArticleId IdType="pubmed">21909514</ArticleId><ArticleId IdType="doi">10.1039/c1cp21964b</ArticleId></ArticleIdList></PubmedData></pubmed></record>Pour manipuler ce document sous Unix (Dilib)
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