Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 114, Issue 12, Pages 3044-3049Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1702510114
Keywords
fluorescence; supramolecular metallacycles; host-guest interactions; white-light emission; orthogonal interactions
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Funding
- National Science Foundation [1212799]
- National Natural Science Foundation of China [21574034, 21274034]
- Zhejiang Provincial Natural Science Foundation of China [LY16B040006]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1212799] Funding Source: National Science Foundation
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Control over the fluorescence of supramolecular assemblies is crucial for the development of chemosensors and light-emitting materials. Consequently, the postsynthetic modification of supramolecular structures via host-guest interactions has emerged as an efficient strategy in recent years that allows the facile tuning of the photophysical properties without requiring a tedious chemical synthesis. Herein, we used a phenanthrene-21-crown-7 (P21C7)-based 60 degrees diplatinum(II) acceptor 8 in the construction of three exohedral P21C7 functionalized rhomboidal metallacycles 1-3 which display orange, cyan, and green emission colors, respectively. Although these colors originate from the dipyridyl precursors 10-12, containing triphenylamine-, tetraphenylethene-, and pyrene-based fluorophores, respectively, the metal-ligand coordination strongly influences their emission properties. The metallacycles were further linked into emissive supramolecular oligomers by the addition of a fluorescent bis-ammonium linker 4 that forms complementary host-guest interactions with the pendant P21C7 units. Notably, the final ensemble derived from a 1: 1 mixture of 1 and 4 displays a concentration-dependent emission. At low concentration, i. e., < 25 mu M, it emits a blue color, whereas an orange emission was observed when the concentration exceeds > 5 mM. Moreover, white-light emission was observed from the same sample at a concentration of 29 mu M, representing a pathway to construct supramolecular assemblies with tunable fluorescence properties.
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