Self‐Assembly of a Giant Molecular Solomon Link from 30 Subcomponents

Schouwey, Clément; Holstein, Julian J.; Scopelliti, Rosario; Zhurov, Konstantin O.; Nagornov, Konstantin O.; Tsybin, Yury O.; Smart, Oliver S.; Bricogne, G.; Severin, Kay

doi:10.1002/anie.201407144

Cited by 90 publications

(42 citation statements)

References 74 publications

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“…The obtained characteristics approach those of the most sophisticated ICR cells with complex approaches to electric field harmonization, either statically or dynamically, for the investigated 10 T magnetic field [24,29,46]. The described NADEL ICR cell has been employed to perform routine mass analysis in our laboratory and demonstrated an ability to achieve the required analytical objectives of molecular structural analysis in a number of applications, for example in the analysis of supramolecular complexes [54].…”

Section: Nadel Icr Cell Performance: Resolving Powermentioning

confidence: 74%

Ion Trap with Narrow Aperture Detection Electrodes for Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Nagornov

Kozhinov

Tsybin

et al. 2015

J. Am. Soc. Mass Spectrom.

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Abstract. The current paradigm in ion trap (cell) design for Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is the ion detection with wide aperture detection electrodes. Specifically, excitation and detection electrodes are typically 90°wide and positioned radially at a similar distance from the ICR cell axis. Here, we demonstrate that ion detection with narrow aperture detection electrodes (NADEL) positioned radially inward of the cell's axis is feasible and advantageous for FT-ICR MS. We describe design details and performance characteristics of a 10 T FT-ICR MS equipped with a NADEL ICR cell having a pair of narrow aperture (flat) detection electrodes and a pair of standard 90°excitation electrodes. Despite a smaller surface area of the detection electrodes, the sensitivity of the NADEL ICR cell is not reduced attributable to improved excite field distribution, reduced capacitance of the detection electrodes, and their closer positioning to the orbits of excited ions. The performance characteristics of the NADEL ICR cell are comparable with the state-of-the-art FT-ICR MS implementations for small molecule, peptide, protein, and petroleomics analyses. In addition, the NADEL ICR cell's design improves the flexibility of ICR cells and facilitates implementation of advanced capabilities (e.g., quadrupolar ion detection for improved mainstream applications). It also creates an intriguing opportunity for addressing the major bottleneck in FTMS-increasing its throughput via simultaneous acquisition of multiple transients or via generation of periodic non-sinusoidal transient signals.

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Section: Nadel Icr Cell Performance: Resolving Powermentioning

confidence: 74%

Ion Trap with Narrow Aperture Detection Electrodes for Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Nagornov

Kozhinov

Tsybin

et al. 2015

J. Am. Soc. Mass Spectrom.

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“…Over the last decades, a variety of interlocked molecules have been created, ranging from Borromean rings, [1][2][3] knots, [4,5] catenanes, [6] rotaxanes, [7] pretzelanes [8,9] to Solomon-links [10] and Daisy-chains. Over the last decades, a variety of interlocked molecules have been created, ranging from Borromean rings, [1][2][3] knots, [4,5] catenanes, [6] rotaxanes, [7] pretzelanes [8,9] to Solomon-links [10] and Daisy-chains.…”

Section: Introductionmentioning

confidence: 99%

DNA Origami Catenanes Templated by Gold Nanoparticles

Peil

Zhan

Liu

2020

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molecule via a transition metal ion and subsequently closed by another crescentshaped molecule in a single cyclization reaction. In strategy B "entwining," two crescent-shaped molecules are linked together via a transition metal ion, followed by a double cyclization reaction to close them at once. In each case, the transition metal ion can be removed after serving its purpose, enabling the free relative movements of the two rings.Mechanically interlocked architectures are appealing building blocks for the realization of many functional devices. Importantly, they empower broad applications in nanomaterials, nanorobotics, and nanomachines. [18][19][20][21] For instance, catenanes have been exploited as switches, [22] rotary motors, [23,24] and sensors. [25][26][27][28][29][30] Rotaxanes have been used as molecular shuttles, [31,32] switches in molecular electronics, [33] control of chemical synthesis, [34] and force-generating components for molecular elevators [35] and pumps. [36] An alternative pathway to create topologically complex molecular architectures is structural DNA nanotechnology, which exploits DNA as both genetic and construction material. [37][38][39][40] The first topological DNA structures were demonstrated by Seeman and co-workers, who synthesized a variety of DNA knots and Borromean rings. [41,42] It was then followed by the construction of DNA catenanes, [43][44][45][46] rotary motors, [47,48] a biohybrid nanoengine, [49] and logic circuits. [50] In 2010, DNA rotaxanes were reported. [51] Subsequently, chemically more rigid, [52] light-switchable, [53] and Daisy-chain rotaxanes, [54] DNA-nanoparticle rotaxanes [55] as well as catalytically active rotaxanes [56] were demonstrated. Despite being topologically well-defined, the as-fabricated DNA catenanes and rotaxanes were in general mechanically rather flexible and floppy, because they were made of single-or doublestranded DNA. By contrast, DNA origami-based interlocked architectures possess much better structural rigidity. The first attempt to realize such catenanes was carried out by Yan and co-workers, who followed an innovative scheme of molecular kirigami. [57] In 2016, Simmel and co-workers reported switchable DNA origami rotaxanes with long-range on-axis motion. [58] In this work, we experimentally demonstrate the hierarchical assembly of DNA origami catenanes templated by gold nanoparticles (AuNPs), taking inspirations from the transition metal-templated synthesis of catenanes developed by Sauvage and co-workers. DNA origami catenanes, which contain two, three or four interlocked rings are successfully created. In particular, the origami rings within the individual catenanes can be set free with respect to one another by releasing the interconnecting AuNPs through toehold-mediated strand displacement reactions.Mechanically interlocked molecules have marked a breakthrough in the field of topological chemistry and boosted the vigorous development of molecular machinery. As an archetypal example of the interlocked molecules, catenanes compri...

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“…A one-pot strategy using a cyclic helicate scaffold to bring the end groups into closer proximity has also been described (Figure 1 b),5d the ligand strands joined through reversible imine formation, which provides a mechanism through which connectivity errors can be corrected 10. Several other Solomon links with metal-bridged5c,5f, 6b,6c,6f or wholly organic6a,6d,6e frameworks have also been isolated. Here we report on the designed synthesis of a Solomon link utilizing an interwoven 2×2 molecular grid to create a crossing point at the site of each metal ion (Figure 1 c).…”

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confidence: 99%

A Solomon Link through an Interwoven Molecular Grid

et al. 2015

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A molecular Solomon link was synthesized through the assembly of an interwoven molecular grid consisting of four bis(benzimidazolepyridyl)benzthiazolo[5,4-d]thiazole ligands and four zinc(II), iron(II), or cobalt(II) cations, followed by ring-closing olefin metathesis. NMR spectroscopy, mass spectrometry, and X-ray crystallography confirmed the doubly interlocked topology, and subsequent demetalation afforded the wholly organic Solomon link. The synthesis, in which each metal ion defines the crossing point of two ligand strands, suggests that interwoven molecular grids should be useful scaffolds for the rational construction of other topologically complex structures.

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Self‐Assembly of a Giant Molecular Solomon Link from 30 Subcomponents

Cited by 90 publications

References 74 publications

Ion Trap with Narrow Aperture Detection Electrodes for Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Ion Trap with Narrow Aperture Detection Electrodes for Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

DNA Origami Catenanes Templated by Gold Nanoparticles

A Solomon Link through an Interwoven Molecular Grid

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