Chiral Conjugated Corrals.

We present here a new design motif for strained, conjugated macrocycles that incorporates two different aromatics into the cycle with an -A-B-A-B- pattern. In this study, we demonstrate the concept by alternating electron donors and acceptors in a conjugated cycle. The donor is a bithiophene, and th...

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Published in:Journal of the American Chemical Society Vol. 137; no. 31; pp. 9982 - 9988
Main Authors: Ball, Melissa, Fowler, Brandon, Panpan Li, Joyce, Leo A., Fang Li, Taifeng Liu, Paley, Daniel, Yu Zhong, Hexing Li, Shengxiong Xiao, Fay Ng, Steigerwald, Michael L., Nuckolls, Colin
Format: Article
Published: American Chemical Society 8/12/2015
Subjects:
Online Access:View this record in EBSCOhost
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      dt: 8/12/2015
      vid: 137
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      pub: American Chemical Society
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        10.1021/jacs.5b05698
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        atl: Chiral Conjugated Corrals.
      aug:
        au:
          Ball, Melissa
          Fowler, Brandon
          Panpan Li
          Joyce, Leo A.
          Fang Li
          Taifeng Liu
          Paley, Daniel
          Yu Zhong
          Hexing Li
          Shengxiong Xiao
          Fay Ng
          Steigerwald, Michael L.
          Nuckolls, Colin
        affil:
          Department of Chemistry, Columbia University, New York, New York 10027, United States
          The Education Ministry Key Lab of Resource Chemistry, Shanghai Key Laboratoiy of Rare Earth Functional Materials, Optoelectronic Nano Materials and Devices Institute, Department of Chemistry, Shanghai Normal University, Shanghai, China 200234
          Process and Analytical Chemistry, Merck Research Laboratories, Rahway, New Jersey 07065, United States
      su:
        Macrocyclic compounds
        Corrals
        Electron donors
        Electrophiles
        Perylene
        Thiophenes
        Chirality
        Density functional theory
      sug:
        subj:
          Macrocyclic compounds
          Corrals
          Electron donors
          Electrophiles
          Perylene
          Thiophenes
          Chirality
          Density functional theory
      ab: We present here a new design motif for strained, conjugated macrocycles that incorporates two different aromatics into the cycle with an -A-B-A-B- pattern. In this study, we demonstrate the concept by alternating electron donors and acceptors in a conjugated cycle. The donor is a bithiophene, and the acceptor is a perylene diimide derivative. The macrocycle formed has a persistent elliptiform cavity that is lined with the sulfur atoms of the thiophenes and the Tt-faces of the perylene diimide. Due to the linkage of the perylene diimide subunits, the macrocycles exist in both chiral and achiral forms. We separate the three stereoisomers using chiral high-performance liquid chromatography and study their interconversion. The mechanism for interconversion involves an "intramolecular somersault" in which one of the PDIs rotates around its transverse axis, thereby moving one of its diimide heads through the plane of the cavity. These unusual macrocycles are black in color with an absorption spectrum that spans the visible range. Density functional theory calculations reveal a photoinduced electron transfer from the bithiophene to the perylene diimide.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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