Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence
Abstract
Predictable stereoselective formation of supramolecular assembly is generally believed to be an important but complicated process. Here, we show that point chirality of a ligand decisively influences its supramolecular assembly behavior. We designed three closely related chiral ligands with different point chiralities, and observe their self-assembly into europium (Eu) tetrametallic tetrahedral cages. One ligand exhibits a highly diastereoselective assembly into homochiral (either ΔΔΔΔ or ΛΛΛΛ) Eu tetrahedral cages whereas the two other ligands, with two different approaches of loosened point chirality, lead to a significant breakdown of the diastereoselectivity to generate a mixture of (ΔΔΔΔ and ΛΛΛΛ) isomers. The cages are highly emissive (luminescence quantum yields of 16(1) to 18(1)%) and exhibit impressive circularly polarized luminescence properties (|g lum |: up to 0.16). With in-depth studies, we present an example that correlates the nonlinear enhancement of the chiroptical response to the nonlinearity dependence on point chirality.
- Authors:
-
[3];
- The Hong Kong Polytechnic Univ., Kowloon (Hong Kong)
- Durham Univ., Durham (United Kingdom)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1419458
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Yeung, Chi -Tung, Yim, King -Him, Wong, Ho -Yin, Pal, Robert, Lo, Wai -Sum, Yan, Siu -Cheong, Yee-Man Wong, Melody, Yufit, Dmitry, Smiles, Danil E., McCormick, Laura J., Teat, Simon J., Shuh, David K., Wong, Wing -Tak, and Law, Ga -Lai. Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence. United States: N. p., 2017.
Web. doi:10.1038/s41467-017-01025-1.
Yeung, Chi -Tung, Yim, King -Him, Wong, Ho -Yin, Pal, Robert, Lo, Wai -Sum, Yan, Siu -Cheong, Yee-Man Wong, Melody, Yufit, Dmitry, Smiles, Danil E., McCormick, Laura J., Teat, Simon J., Shuh, David K., Wong, Wing -Tak, & Law, Ga -Lai. Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence. United States. https://doi.org/10.1038/s41467-017-01025-1
Yeung, Chi -Tung, Yim, King -Him, Wong, Ho -Yin, Pal, Robert, Lo, Wai -Sum, Yan, Siu -Cheong, Yee-Man Wong, Melody, Yufit, Dmitry, Smiles, Danil E., McCormick, Laura J., Teat, Simon J., Shuh, David K., Wong, Wing -Tak, and Law, Ga -Lai. Tue .
"Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence". United States. https://doi.org/10.1038/s41467-017-01025-1. https://www.osti.gov/servlets/purl/1419458.
@article{osti_1419458,
title = {Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence},
author = {Yeung, Chi -Tung and Yim, King -Him and Wong, Ho -Yin and Pal, Robert and Lo, Wai -Sum and Yan, Siu -Cheong and Yee-Man Wong, Melody and Yufit, Dmitry and Smiles, Danil E. and McCormick, Laura J. and Teat, Simon J. and Shuh, David K. and Wong, Wing -Tak and Law, Ga -Lai},
abstractNote = {Predictable stereoselective formation of supramolecular assembly is generally believed to be an important but complicated process. Here, we show that point chirality of a ligand decisively influences its supramolecular assembly behavior. We designed three closely related chiral ligands with different point chiralities, and observe their self-assembly into europium (Eu) tetrametallic tetrahedral cages. One ligand exhibits a highly diastereoselective assembly into homochiral (either ΔΔΔΔ or ΛΛΛΛ) Eu tetrahedral cages whereas the two other ligands, with two different approaches of loosened point chirality, lead to a significant breakdown of the diastereoselectivity to generate a mixture of (ΔΔΔΔ and ΛΛΛΛ) isomers. The cages are highly emissive (luminescence quantum yields of 16(1) to 18(1)%) and exhibit impressive circularly polarized luminescence properties (|g lum |: up to 0.16). With in-depth studies, we present an example that correlates the nonlinear enhancement of the chiroptical response to the nonlinearity dependence on point chirality.},
doi = {10.1038/s41467-017-01025-1},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Tue Oct 24 00:00:00 EDT 2017},
month = {Tue Oct 24 00:00:00 EDT 2017}
}
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Figures / Tables:
Fig. 1: Self-assembly of tetrahedral cages. a Ligands (L= L1–L3) used for studying the stereoselective formation behavior of the tetrahedral cages. b A projecture of the stereoselective formation of the tetrahedral cage Λ,Λ,Λ,Λ-[Eu4(L1RR)6](OTf)12]. Cavity for potential encapsulation of guest molecules is highlighted as a yellow spherical space. c Energy-minimized schematicmore »
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