Meissner, Stefanie A. and Eder, Theresa and Keller, Tristan J. and Hofmeister, David A. and Spicher, Sebastian and Jester, Stefan-S and Vogelsang, Jan and Grimme, Stefan and Lupton, John M. and Hoeger, Sigurd (2021) Nanoscale pi-conjugated ladders. NATURE COMMUNICATIONS, 12 (1): 6614. ISSN 2041-1723
Full text not available from this repository. (Request a copy)Abstract
Increasing the rigidity of a macromolecule while maintaining solubility is challenging. Here, the authors demonstrate covalent connection of two rigid-rod polymer chains with stiff connectors, leading to rigid ladder structures with well-defined conjugated rails. It is challenging to increase the rigidity of a macromolecule while maintaining solubility. Established strategies rely on templating by dendrons, or by encapsulation in macrocycles, and exploit supramolecular arrangements with limited robustness. Covalently bonded structures have entailed intramolecular coupling of units to resemble the structure of an alternating tread ladder with rungs composed of a covalent bond. We introduce a versatile concept of rigidification in which two rigid-rod polymer chains are repeatedly covalently associated along their contour by stiff molecular connectors. This approach yields almost perfect ladder structures with two well-defined pi-conjugated rails and discretely spaced nanoscale rungs, easily visualized by scanning tunnelling microscopy. The enhancement of molecular rigidity is confirmed by the fluorescence depolarization dynamics and complemented by molecular-dynamics simulations. The covalent templating of the rods leads to self-rigidification that gives rise to intramolecular electronic coupling, enhancing excitonic coherence. The molecules are characterized by unprecedented excitonic mobility, giving rise to excitonic interactions on length scales exceeding 100 nm. Such interactions lead to deterministic single-photon emission from these giant rigid macromolecules, with potential implications for energy conversion in optoelectronic devices.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | EXCITON LOCALIZATION; ENERGY-TRANSFER; POLYMER-CHAINS; CHROMOPHORES; STATE |
| Subjects: | 500 Science > 530 Physics |
| Divisions: | Physics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 05 Jul 2022 05:39 |
| Last Modified: | 05 Jul 2022 05:39 |
| URI: | https://pred.uni-regensburg.de/id/eprint/46852 |
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