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A unique non-catenane interlocked self-assembled supramolecular architecture and its photophysical properties.

ABSTRACT: A novel, interlocked, self-assembled (M(2)L(2))(2) molecular architecture was constructed from an arene-Ru acceptor and a 1,4-di(pyridin-4-yl)buta-1,3-diyne donor. Two M(2)L(2) units, with cavities of ~7.21 Å, spontaneously interlock, with one unit encapsulating a twin in a non-catenane fashion. The dimeric host-guest complex thus formed is unique among two-dimensional self-assemblies and is stabilized by ?-? interactions between the M(2)L(2) units.

SUBMITTER: Vajpayee V

PROVIDER: S-EPMC3235908 | biostudies-literature | 2011 Dec

REPOSITORIES: biostudies-literature

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A unique non-catenane interlocked self-assembled supramolecular architecture and its photophysical properties.

Vajpayee Vaishali V Song Young Ho YH Cook Timothy R TR Kim Hyunuk H Lee Youngil Y Stang Peter J PJ Chi Ki-Whan KW

Journal of the American Chemical Society 20111115 49

A novel, interlocked, self-assembled (M(2)L(2))(2) molecular architecture was constructed from an arene-Ru acceptor and a 1,4-di(pyridin-4-yl)buta-1,3-diyne donor. Two M(2)L(2) units, with cavities of ~7.21 Å, spontaneously interlock, with one unit encapsulating a twin in a non-catenane fashion. The dimeric host-guest complex thus formed is unique among two-dimensional self-assemblies and is stabilized by π-π interactions between the M(2)L(2) units. ...[more]

PMID: 22085308

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Project description:In the present study, the influence of the hydrogen bonding for the one- and two-photon absorption of the prototypical squaraine dye is investigated with quantum chemistry tools. The central squaraine unit is bound by strong hydrogen bonds with 4-substituted N,N'-diphenylurea and, alternatively, N,N'-diphenylthiourea molecules, which affects to a high extend the properties of the squaraine electron accepting moiety, thus shifting its maximum absorption wavelength and enhancing the TPA cross section. The replacement of oxygen by sulfur atoms in the squaraine central ring, known to affect its photophysical behavior, is considered here as the way of modifying the strength and nature of the intermolecular contacts. Additionally, the influence of the oxygen-by-sulfur replacement is also considered in the N,N'-diphenylurea moiety, as the factor affecting the acidity of the N-H protons. The introduction of the sequence of the substituents of varying electron-donating or electron-withdrawing characters in the position 4 of N,N'-diphenyl(thio)urea subsystems allows to finely tune the hydrogen bonding with the central squaraine unit by further modification of the N-H bond characteristics. All of these structural modifications lead to the controlled adjustment of the electron density distribution, and thus, the properties affected such as transition moments and absorption intensity. Ab initio calculations provide strong support for this way of tailoring of one- or two-photon absorption due to the obtained strong hypsochromic shift of the maximum one-photon absorption wavelength observed particularly for thiosquaraine complexes and an increase in the TPA wavelength together with the increase in the TPA cross section. Moreover, the source of the strong modification of the thiosquaraine OPA in contrast to the pristine oxosquaraine upon N,N'-diphenyl(thio)urea substitution is determined. Furthermore, for the first time, the linear dependence of the non-additivity in the interaction energy on the Hammett substituent constant is reported. The stronger the electron-donating character of the substituent, the larger the three-body non-additive components and the larger their percentage to the total interaction energy.

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A unique non-catenane interlocked self-assembled supramolecular architecture and its photophysical properties.

Publications

A unique non-catenane interlocked self-assembled supramolecular architecture and its photophysical properties.

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