Molecular Control of Internal Crystallization and Photocatalytic Function in Supramolecular Nanostructures.
| Autor: | Kazantsev RV; Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.; Argonne Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, IL 60208, USA., Dannenhoffer A; Department of Materials Science and Engineering, Evanston, IL 60208, USA., Aytun T; Department of Materials Science and Engineering, Evanston, IL 60208, USA., Harutyunyan B; Argonne Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, IL 60208, USA.; Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208, USA., Fairfield DJ; Department of Materials Science and Engineering, Evanston, IL 60208, USA., Bedzyk MJ; Department of Materials Science and Engineering, Evanston, IL 60208, USA.; Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208, USA., Stupp SI; Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.; Argonne Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, IL 60208, USA.; Department of Materials Science and Engineering, Evanston, IL 60208, USA.; Department of Medicine, Northwestern University, Chicago, IL 60611, USA.; Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, IL 60611, USA.; Department of Biomedical Engineering, Northwestern University, Evanston, IL 60208, USA.; Lead Contact. |
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| Jazyk: | angličtina |
| Zdroj: | Chem [Chem] 2018 Jul 12; Vol. 4 (7), pp. 1596-1608. Date of Electronic Publication: 2018 May 03. |
| DOI: | 10.1016/j.chempr.2018.04.002 |
| Abstrakt: | Supramolecular light-absorbing nanostructures are useful building blocks for the design of next-generation artificial photosynthetic systems. Development of such systems requires a detailed understanding of how molecular packing influences the material's optoelectronic properties. We describe a series of crystalline supramolecular nanostructures in which the substituents on their monomeric units strongly affects morphology, ordering kinetics, and exciton behavior. By designing constitutionally-isomeric perylene monoimide (PMI) amphiphiles, the effect of side chain sterics on nanostructure crystallization was studied. Molecules with short amine linked alkyl-tails rapidly crystallize upon dissolution in water, while bulkier tails require the addition of salt to screen electrostatic repulsion and annealing to drive crystallization. A PMI monomer bearing a 3-pentylamine tail was found to possess a unique structure that results in strongly red-shifted absorbance, indicative of charge-transfer exciton formation. This particular supramolecular structure was found to have an enhanced ability to photosensitize a thiomolybdate, [(NH |
| Databáze: | MEDLINE |
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