Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence

Chi Tung Yeung; King Him Yim; Ho Yin Wong; Robert Pal; Wai Sum Lo; Siu Cheong Yan; Melody Yee Man Wong; Dmitry Yufit; Danil E. Smiles; Laura J. McCormick; Simon J. Teat; David K. Shuh; Wing Tak Wong; Ga Lai Law

doi:10.1038/s41467-017-01025-1

Chiral transcription in self-assembled tetrahedral Eu₄L₆ chiral cages displaying sizable circularly polarized luminescence

Chi Tung Yeung, King Him Yim, Ho Yin Wong, Robert Pal, Wai Sum Lo, Siu Cheong Yan, Melody Yee Man Wong, Dmitry Yufit, Danil E. Smiles, Laura J. McCormick, Simon J. Teat, David K. Shuh, Wing Tak Wong^*, Ga Lai Law^*

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Journal article › peer-review

132 Citations (Scopus)

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.

Original language	English
Article number	1128
Journal	Nature Communications
Volume	8
Early online date	24 Oct 2017
DOIs	https://doi.org/10.1038/s41467-017-01025-1
Publication status	Published - Dec 2017

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Yeung, C. T., Yim, K. H., Wong, H. Y., Pal, R., Lo, W. S., Yan, S. C., Wong, M. Y. M., Yufit, D., Smiles, D. E., McCormick, L. J., Teat, S. J., Shuh, D. K., Wong, W. T., & Law, G. L. (2017). Chiral transcription in self-assembled tetrahedral Eu₄L₆ chiral cages displaying sizable circularly polarized luminescence. Nature Communications, 8, Article 1128. https://doi.org/10.1038/s41467-017-01025-1

@article{54881449f143428eaf3c879e29e6675d,

title = "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.",

author = "Yeung, {Chi Tung} and Yim, {King Him} and Wong, {Ho Yin} and Robert Pal and Lo, {Wai Sum} and Yan, {Siu Cheong} and Wong, {Melody Yee Man} and Dmitry Yufit and Smiles, {Danil E.} and McCormick, {Laura J.} and Teat, {Simon J.} and Shuh, {David K.} and Wong, {Wing Tak} and Law, {Ga Lai}",

note = "Funding information: This paper is dedicated to Professor Kenneth N. Raymond on the occasion of his 75th birthday. We gratefully acknowledge the funding from The Hong Kong Polytechnic University [University Research Facility for Chemical and Environmental Analysis (UCEA), Area of Excellence Grants (1-ZVGG)], Hong Kong Research Grants Council (Collaborative Research Grants, CRF PolyU11/CRF/13E), the Basic Research Program of Shenzhen (No. JCYJ20160531184120814) and The Hong Kong Polytechnic University. (PolyU 5096/13P). H.-Y.W. acknowledges the postgraduate studentship from the Hong Kong Polytechnic University. Parts of this work (D.E.S., D.K.S.). were supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences Heavy Element Chemistry Program of the U.S. Department of Energy at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231 and supported the efforts of L.J.M. and S.J.T. R.P. acknowledge the Royal Society URF for funding and Ms. Holly V. Linford for the help with the CPL measurements. Publisher copyright: {\textcopyright} The Author(s) 2017",

year = "2017",

month = dec,

doi = "10.1038/s41467-017-01025-1",

language = "English",

volume = "8",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

}

TY - JOUR

T1 - Chiral transcription in self-assembled tetrahedral Eu4L6 chiral cages displaying sizable circularly polarized luminescence

AU - Yeung, Chi Tung

AU - Yim, King Him

AU - Wong, Ho Yin

AU - Pal, Robert

AU - Lo, Wai Sum

AU - Yan, Siu Cheong

AU - Wong, Melody Yee Man

AU - Yufit, Dmitry

AU - Smiles, Danil E.

AU - McCormick, Laura J.

AU - Teat, Simon J.

AU - Shuh, David K.

AU - Wong, Wing Tak

AU - Law, Ga Lai

N1 - Funding information: This paper is dedicated to Professor Kenneth N. Raymond on the occasion of his 75th birthday. We gratefully acknowledge the funding from The Hong Kong Polytechnic University [University Research Facility for Chemical and Environmental Analysis (UCEA), Area of Excellence Grants (1-ZVGG)], Hong Kong Research Grants Council (Collaborative Research Grants, CRF PolyU11/CRF/13E), the Basic Research Program of Shenzhen (No. JCYJ20160531184120814) and The Hong Kong Polytechnic University. (PolyU 5096/13P). H.-Y.W. acknowledges the postgraduate studentship from the Hong Kong Polytechnic University. Parts of this work (D.E.S., D.K.S.). were supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences Heavy Element Chemistry Program of the U.S. Department of Energy at Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231 and supported the efforts of L.J.M. and S.J.T. R.P. acknowledge the Royal Society URF for funding and Ms. Holly V. Linford for the help with the CPL measurements. Publisher copyright: © The Author(s) 2017

PY - 2017/12

Y1 - 2017/12

N2 - 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.

AB - 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.

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U2 - 10.1038/s41467-017-01025-1

DO - 10.1038/s41467-017-01025-1

M3 - Journal article

SN - 2041-1723

VL - 8

JO - Nature Communications

JF - Nature Communications

M1 - 1128

ER -

Chiral transcription in self-assembled tetrahedral Eu₄L₆ chiral cages displaying sizable circularly polarized luminescence

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