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Conventional approaches to the synthesis of molecular knots and links mostly rely on metal templation. We present here an alternative strategy that uses the hydrophobic effect to drive the formation of complex interlocked structures in water. We designed an aqueous dynamic combinatorial system that can generate knots and links. In this system, the self-assembly of a topologically complex macrocycle is thermodynamically favored only if an optimum packing of all its components minimizes the hydrophobic surface area in contact with water. Therefore, the size, geometry, and rigidity of the initial building blocks can be exploited to control the formation of a specific topology. We illustrate the validity of this concept with the syntheses of a Hopf link, a Solomon link, and a trefoil knot. This latter molecule, whose self-assembly is templated by halides, binds iodide with high affinity in water. Overall, this work brings a fresh perspective on the synthesis of topologically complex molecules: Solvophobic effects can be intentionally harnessed to direct the efficient and selective self-assembly of knots and links.
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http://dx.doi.org/10.1021/jacs.8b05220 | DOI Listing |
Phys Rev Lett
December 2024
CAS Key Laboratory of Quantum Information, University of Science and Technology of China, Hefei 230026, China.
By braiding non-Abelian anyons it is possible to realize fault-tolerant quantum algorithms through the computation of Jones polynomials. So far, this has been an experimentally formidable task. In this Letter, a photonic quantum system employing two-photon correlations and nondissipative imaginary-time evolution is utilized to simulate two inequivalent braiding operations of Majorana zero modes.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
QCD Labs, QTF Centre of Excellence, Department of Applied Physics, Aalto University, P.O. Box 13500, FI-00076 Aalto, Finland.
Ordered media often support vortex structures with intriguing topological properties. Here, we investigate non-Abelian vortices in tetrahedral order using the mathematical formalism of colored links. Due to the generality of our methods, the results apply to all physical systems governed by tetrahedral order, such as the cyclic phase of spin-2 Bose-Einstein condensates and the tetrahedratic phase of bent-core nematic liquid crystals.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
University of Wroclaw: Uniwersytet Wroclawski, Chemistry, 14 F. Joliot-Curie 14, 50383, Wroclaw, POLAND.
A subtle interplay between the flexibility of the 2,2'-bipyridyl-based diamine and the denticity of the coordination domain formed upon self-assembly enabled the formation of four distinct topologies stabilised by [Ag···Ag]2+ pairs. The reactions utilising 2,6-diformylpyridine resulted in the formation of silver(I)-stabilised molecular tweezer, trefoil knot, and Solomon link. The 1,8-naphthyridine-based dialdehyde promoted the formation of [2]catenanes and trefoil knot, demonstrating very close AgI···AgI distances.
View Article and Find Full Text PDFAdv Sci (Weinh)
December 2024
Department of Geriatric Dentistry, Beijing Laboratory of Biomedical Materials, Peking University School and Hospital of Stomatology, Beijing, 100081, P. R. China.
Proc Natl Acad Sci U S A
October 2024
Department of Mathematics, Michigan State University, East Lansing, MI 48824.
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