PittsburghV1, France, Analysis, bibRecord, 000619

Optimizing sensitization processes in dinuclear luminescent lanthanide oligomers: selection of rigid aromatic spacers.

Identifieur interne : 000619 ( France/Analysis ); précédent : 000618; suivant : 000620

Optimizing sensitization processes in dinuclear luminescent lanthanide oligomers: selection of rigid aromatic spacers.

Auteurs : Jean-François Lemonnier [France] ; Laure Guénée ; César Beuchat [Suisse] ; Tomasz A. Wesolowski ; Prasun Mukherjee ; David H. Waldeck ; Kristy A. Gogick [États-Unis] ; Stéphane Petoud [France] ; Claude Piguet [France]

Source :

Journal of the American Chemical Society [ 0002-7863 ] ; 2011-10-12.

RBID : Hal:hal-00720638

English descriptors

mix :
- AQUO IONS, BOND-VALENCE PARAMETERS, COORDINATION-COMPLEXES, ELECTRONIC ENERGY LEVELS, EUROPIUM, LIGANDS, LIGHT-EMITTING-DIODES, POLYNUCLEAR COMPLEXES, SPECTROSCOPIC PROPERTIES, STERIC CONSTRAINTS.

Abstract

This work illustrates a simple approach for optimizing the lanthanide luminescence in molecular dinuclear lanthanide complexes and identifies a particular multidentate europium complex as the best candidate for further incorporation into polymeric materials. The central phenyl ring in the bis-tridentate model ligands L3-L5, which are substituted with neutral (X = H, L3), electron-withdrawing (X = F, L4), or electron-donating (X = OCH3, L5) groups, separates the 2,6-bis(benzimidazol-2-yl)pyridine binding units of linear oligomeric multi-tridentate ligand strands that are designed for the complexation of luminescent trivalent lanthanides, Ln(III). Reactions of L3-L5 with [Ln(hfac)3(diglyme)] (hfac- is the hexafluoroacetylacetonate anion) produce saturated single-stranded dumbbell-shaped complexes [Ln2(Lk)(hfac)6] (k = 3-5), in which the lanthanide ions of the two nine-coordinate neutral [N3Ln(hfac)3] units are separated by 12-14 Å. The thermodynamic affinities of [Ln(hfac)3] for the tridentate binding sites in L3-L5 are average (6.6 ≤ log(β(2,1)(Y,Lk)) ≤ 8.4) but still result in 15-30% dissociation at millimolar concentrations in acetonitrile. In addition to the empirical solubility trend found in organic solvents (L4 > L3 > L5), which suggests that the 1,4-difluorophenyl spacer in L4 is preferable, we have developed a novel tool for deciphering the photophysical sensitization processes operating in [Eu2(Lk)(hfac)6]. A simple interpretation of the complete set of rate constants characterizing the energy migration mechanisms provides straightforward objective criteria for the selection of [Eu2(L4)(hfac)6] as the most promising building block.

Url:

https://hal.archives-ouvertes.fr/hal-00720638

DOI: 10.1021/ja206806t

Affiliations:

Links toward previous steps (curation, corpus...)

to stream Hal, to step Corpus: 000446
to stream Hal, to step Curation: 000446
to stream Hal, to step Checkpoint: 000395
to stream Main, to step Merge: 00A311
to stream Main, to step Curation: 009B66
to stream Main, to step Exploration: 009B66
to stream France, to step Extraction: 000619

Links to Exploration step

Hal:hal-00720638

Le document en format XML

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<author><name sortKey="Piguet, Claude" sort="Piguet, Claude" uniqKey="Piguet C" first="Claude" last="Piguet">Claude Piguet</name>
<affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-14457" status="VALID">          <idno type="IdRef">189548800</idno>
          <idno type="ISNI">0000 0004 0368 2940</idno>
          <idno type="RNSR">200612827W</idno>
          <orgName>Institut Lavoisier de Versailles</orgName>
          <orgName type="acronym">ILV</orgName>
          <date type="start">2006</date>
          <desc>            <address>              <addrLine>Bâtiment Lavoisier 45 avenue des Etats Unis 78035 VERSAILLES CEDEX</addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.ilv.uvsq.fr/</ref>
          </desc>
          <listRelation>            <relation name="UMR8180" active="#struct-81173" type="direct"></relation>
            <relation name="UMR8180" active="#struct-441569" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle name="UMR8180" active="#struct-81173" type="direct"><org type="institution" xml:id="struct-81173" status="VALID">          <idno type="IdRef">03082057X</idno>
          <idno type="ISNI">0000 0001 2323 0229 </idno>
          <orgName>Université de Versailles Saint-Quentin-en-Yvelines</orgName>
          <orgName type="acronym">UVSQ</orgName>
          <date type="start">1991-07-22</date>
          <desc>            <address>              <addrLine>55 avenue de Paris - 78035 Versailles cedex</addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.uvsq.fr/</ref>
          </desc>
        </org>
</tutelle>
<tutelle name="UMR8180" active="#struct-441569" type="direct"><org type="institution" xml:id="struct-441569" status="VALID">          <idno type="IdRef">02636817X</idno>
          <idno type="ISNI">0000000122597504</idno>
          <orgName>Centre National de la Recherche Scientifique</orgName>
          <orgName type="acronym">CNRS</orgName>
          <date type="start">1939-10-19</date>
          <desc>            <address>              <country key="FR"></country>
            </address>
            <ref type="url">http://www.cnrs.fr/</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>France</country>
<placeName><settlement type="city">Versailles</settlement>
<region type="region" nuts="2">Île-de-France</region>
</placeName>
<orgName type="university">Université de Versailles-Saint-Quentin-en-Yvelines</orgName>
</affiliation>
</author>
</analytic>
<idno type="DOI">10.1021/ja206806t</idno>
<series><title level="j">Journal of the American Chemical Society</title>
<idno type="ISSN">0002-7863</idno>
<imprint><date type="datePub">2011-10-12</date>
</imprint>
</series>
</biblStruct>
</sourceDesc>
</fileDesc>
<profileDesc><textClass><keywords scheme="mix" xml:lang="en"><term>AQUO IONS</term>
<term>BOND-VALENCE PARAMETERS</term>
<term>COORDINATION-COMPLEXES</term>
<term>ELECTRONIC ENERGY LEVELS</term>
<term>EUROPIUM</term>
<term>LIGANDS</term>
<term>LIGHT-EMITTING-DIODES</term>
<term>POLYNUCLEAR COMPLEXES</term>
<term>SPECTROSCOPIC PROPERTIES</term>
<term>STERIC CONSTRAINTS</term>
</keywords>
</textClass>
</profileDesc>
</teiHeader>
<front><div type="abstract" xml:lang="en">This work illustrates a simple approach for optimizing the lanthanide luminescence in molecular dinuclear lanthanide complexes and identifies a particular multidentate europium complex as the best candidate for further incorporation into polymeric materials. The central phenyl ring in the bis-tridentate model ligands L3-L5, which are substituted with neutral (X = H, L3), electron-withdrawing (X = F, L4), or electron-donating (X = OCH3, L5) groups, separates the 2,6-bis(benzimidazol-2-yl)pyridine binding units of linear oligomeric multi-tridentate ligand strands that are designed for the complexation of luminescent trivalent lanthanides, Ln(III). Reactions of L3-L5 with [Ln(hfac)3(diglyme)] (hfac- is the hexafluoroacetylacetonate anion) produce saturated single-stranded dumbbell-shaped complexes [Ln2(Lk)(hfac)6] (k = 3-5), in which the lanthanide ions of the two nine-coordinate neutral [N3Ln(hfac)3] units are separated by 12-14 Å. The thermodynamic affinities of [Ln(hfac)3] for the tridentate binding sites in L3-L5 are average (6.6 ≤ log(β(2,1)(Y,Lk)) ≤ 8.4) but still result in 15-30% dissociation at millimolar concentrations in acetonitrile. In addition to the empirical solubility trend found in organic solvents (L4 > L3 > L5), which suggests that the 1,4-difluorophenyl spacer in L4 is preferable, we have developed a novel tool for deciphering the photophysical sensitization processes operating in [Eu2(Lk)(hfac)6]. A simple interpretation of the complete set of rate constants characterizing the energy migration mechanisms provides straightforward objective criteria for the selection of [Eu2(L4)(hfac)6] as the most promising building block.</div>
</front>
</TEI>
<affiliations><list><country><li>France</li>
<li>Suisse</li>
<li>États-Unis</li>
</country>
<region><li>Centre-Val de Loire</li>
<li>Pennsylvanie</li>
<li>Région Centre</li>
<li>Île-de-France</li>
</region>
<settlement><li>Orléans</li>
<li>Pittsburgh</li>
<li>Versailles</li>
</settlement>
<orgName><li>Centre Val de Loire Université</li>
<li>Université d'Orléans</li>
<li>Université de Pittsburgh</li>
<li>Université de Versailles-Saint-Quentin-en-Yvelines</li>
</orgName>
</list>
<tree><noCountry><name sortKey="Guenee, Laure" sort="Guenee, Laure" uniqKey="Guenee L" first="Laure" last="Guénée">Laure Guénée</name>
<name sortKey="Mukherjee, Prasun" sort="Mukherjee, Prasun" uniqKey="Mukherjee P" first="Prasun" last="Mukherjee">Prasun Mukherjee</name>
<name sortKey="Waldeck, David H" sort="Waldeck, David H" uniqKey="Waldeck D" first="David H" last="Waldeck">David H. Waldeck</name>
<name sortKey="Wesolowski, Tomasz A" sort="Wesolowski, Tomasz A" uniqKey="Wesolowski T" first="Tomasz A" last="Wesolowski">Tomasz A. Wesolowski</name>
</noCountry>
<country name="France"><region name="Île-de-France"><name sortKey="Lemonnier, Jean Francois" sort="Lemonnier, Jean Francois" uniqKey="Lemonnier J" first="Jean-François" last="Lemonnier">Jean-François Lemonnier</name>
</region>
<name sortKey="Petoud, Stephane" sort="Petoud, Stephane" uniqKey="Petoud S" first="Stéphane" last="Petoud">Stéphane Petoud</name>
<name sortKey="Piguet, Claude" sort="Piguet, Claude" uniqKey="Piguet C" first="Claude" last="Piguet">Claude Piguet</name>
</country>
<country name="Suisse"><noRegion><name sortKey="Beuchat, Cesar" sort="Beuchat, Cesar" uniqKey="Beuchat C" first="César" last="Beuchat">César Beuchat</name>
</noRegion>
</country>
<country name="États-Unis"><region name="Pennsylvanie"><name sortKey="Gogick, Kristy A" sort="Gogick, Kristy A" uniqKey="Gogick K" first="Kristy A" last="Gogick">Kristy A. Gogick</name>
</region>
</country>
</tree>
</affiliations>
</record>

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Optimizing sensitization processes in dinuclear luminescent lanthanide oligomers: selection of rigid aromatic spacers.

Optimizing sensitization processes in dinuclear luminescent lanthanide oligomers: selection of rigid aromatic spacers.

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