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 (2017) 'Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence.', Nature communications., 8 (1). p. 1128.
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 (|glum|: 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.
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|Publisher Web site:||https://doi.org/10.1038/s41467-017-01025-1|
|Publisher statement:||Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.|
|Date accepted:||11 August 2017|
|Date deposited:||07 November 2017|
|Date of first online publication:||24 October 2017|
|Date first made open access:||07 November 2017|
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