Jump to main content
Jump to site search

Issue 2, 2017
Previous Article Next Article

Design of multi-functional 2D open-shell organic networks with mechanically controllable properties

Author affiliations

Abstract

Triarylmethyls (TAMs) are prominent highly attractive open shell organic molecular building blocks for materials science, having been used in breakthrough syntheses of organic magnetic polymers and metal organic frameworks. With their radical π-conjugated nature and a proven capacity to possess high stability via suitable chemical design, TAMs display a variety of desirable characteristics which can be exploited for a wide range of applications. Due to their particular molecular and electronic structure, the spin localization in TAMs almost entirely depends on the dihedral angles of their three aryl rings with respect to the central methyl carbon atom plane, which opens up the possibility of controlling their fundamental properties by twisting the three aryl rings. Aryl ring twist angles can be tuned to a single value by specific chemical functionalisation but controlling them by external means in organic materials or devices represents a challenging task which has not yet been experimentally achieved. Herein, through rational chemical design we propose two 2D covalent organic frameworks (2D-COFs) based on specific TAM building blocks. By employing ab initio computational modeling we demonstrate that it is possible to externally manipulate the aryl ring twist angles in these 2D-linked TAM frameworks by external mechanical means. Furthermore, we show this structural manipulation allows for finely tuning the most important characteristics of these materials such as spin localization, optical electronic transitions and magnetic interactions. Due to the enormous technological potential offered by this new class of material and the fact that our work is guided by real advances in organic materials synthesis, we believe that our predictions will inspire the experimental realization of radical-2D-COFs with externally controllable characteristics.

Graphical abstract: Design of multi-functional 2D open-shell organic networks with mechanically controllable properties

Back to tab navigation

Supplementary files

Publication details

The article was received on 30 Mar 2016, accepted on 30 Aug 2016 and first published on 31 Aug 2016


Article type: Edge Article
DOI: 10.1039/C6SC01412G
Citation: Chem. Sci., 2017,8, 1027-1039
  • Open access: Creative Commons BY license
  •   Request permissions

    Design of multi-functional 2D open-shell organic networks with mechanically controllable properties

    I. Alcón, D. Reta, I. D. P. R. Moreira and S. T. Bromley, Chem. Sci., 2017, 8, 1027
    DOI: 10.1039/C6SC01412G

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements