Journal
ACS NANO
Volume 15, Issue 2, Pages 2753-2761Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c08539
Keywords
upconverted circularly polarized luminescence; self-assembly; symmetry breaking; photon upconversion; upconversion nanoparticle
Categories
Funding
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB36000000]
- Ministry of Science and Technology of the People's Republic of China [2016YFA0203400, 2017YFA0206600]
- National Natural Science Foundation of China [51673050, 91856115]
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A general supramolecular coassembly approach was developed for fabricating upconverted circularly polarized luminescence systems from completely achiral components, inducing UC-CPL activity through the formation of a chiral nanohelix via symmetry breaking. The research demonstrated that chiral molecules are not required for the fabrication of UC-CPL materials, and the polarization of UC-CPL can be tuned by the helicity of the nanohelix.
Enormous attention has been paid to upconverted circularly polarized luminescence (UC-CPL). However, so far, chiral species are still needed in UC-CPL materials, either through the covalent or noncovalent bond. Here, we report a general supramolecular coassembly approach for the fabrication of UC-CPL systems from completely achiral components. We have found that an achiral C-3-symmetric molecule could form a chiral nanohelix through symmetry breaking, which could serve as a general helical platform to endow achiral guests with induced chirality and CPL activity. Two different photon upconversion systems, namely, triplet-triplet annihilation photon upconversion (TTA-UC) donor/acceptor pairs and inorganic lanthanide upconversion nanoparticles (UCNPs), are selected. When these two systems coassembled with the chiral nanohelix made from an achiral C-3-symmetric molecule, hybrid nanohelix structures formed and UC-CPL activity was induced. Through such an approach, we demonstrated that the fabrication of the UC-CPL materials does not require any chiral molecules. Moreover, we have shown that the polarization of UC-CPL can be tuned by the helicity of the nanohelix, which could be controlled through the seeded vortex. Our work provides a general approach for designing tunable UC-CPL materials from completely achiral motifs, which largely expands the research scope of the CPL materials.
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