Hybrid Organic–Inorganic Rotaxanes, Including a Hetero‐Hybrid [3]Rotaxane Featuring Two Distinct Heterometallic Rings and a Molecular Shuttle

Timco, Grigore A.; Fernández, Antonio; Kostopoulos, Andreas K.; Charlton, Jodie F.; Lockyer, Selena J.; Hailes, Thomas R.; Adams, Ralph W.; McInnes, Eric J. L.; Tuna, Floriana; Vitórica-Yrezábal, Iñigo J.; Whitehead, George F. S.; Winpenny, Richard E. P.

doi:10.1002/anie.201805439

Cited by 25 publications

(23 citation statements)

References 25 publications

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“…This is a problem but also offers some potential in that if we could orientate an array of molecules of 3 we may be able to selectively address specific qubit–qubit interactions and not others. This is immensely ambitious but achievable if we can make diamagnetic equivalents of 3 ; we are developing diamagnetic hybrid rotaxanes for that end 60 , but have not yet achieved assemblies as complex as 3 .…”

Section: Resultsmentioning

confidence: 99%

A [13]rotaxane assembled via a palladium molecular capsule

et al. 2019

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Molecules that are the size of small proteins are difficult to make. The most frequently examined route is via self-assembly, and one particular approach involves molecular nanocapsules, where ligands are designed that will enforce the formation of specific polyhedra of metals within the core of the structure. Here we show that this approach can be combined with mechanically interlocking molecules to produce nanocapsules that are decorated on their exterior. This could be a general route to very large molecules, and is exemplified here by the synthesis and structural characterization of a [13]rotaxane, containing 150 metal centres. Small angle X-ray scattering combined with atomistic molecular dynamics simulations demonstrate the compound is intact in solution.

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Section: Resultsmentioning

confidence: 99%

A [13]rotaxane assembled via a palladium molecular capsule

et al. 2019

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“…It may be possible to overcome this by exploiting broad-band excitation methods enabled by pulse shaping technologies. 41 We are also currently designing Cu···{Cr 7 Ni} rotaxanes with longer and more rigid linkers that should put the interaction energy in the range appropriate for RIDME experiments, and diamagnetic analogues 42 that will allow such experiments on aligned single crystals. 43…”

Section: Discussionmentioning

confidence: 99%

Close Encounters of the Weak Kind: Investigations of Electron–Electron Interactions between Dissimilar Spins in Hybrid Rotaxanes

et al. 2019

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We report a family of hybrid [2]rotaxanes based on inorganic [Cr7NiF8(O2CtBu)16]− (“{Cr7Ni}”) rings templated about organic threads that are terminated at one end with pyridyl groups. These rotaxanes can be coordinated to [Cu(hfac)2] (where Hhfac = 1,1,1,5,5,5-hexafluoroacetylacetone), to give 1:1 or 1:2 Cu:{Cr7Ni} adducts: {[Cu(hfac)2](py-CH2NH2CH2CH2Ph)[Cr7NiF8(O2CtBu)16]}, {[Cu(hfac)2][py-CH2NH2CH2CH3][Cr7NiF8(O2CtBu)16]}, {[Cu(hfac)2]([py-CH2CH2NH2CH2C6H4SCH3][Cr7NiF8(O2CtBu)16])2}, {[Cu(hfac)2]([py-C6H4-CH2NH2(CH2)4Ph][Cr7NiF8(O2CtBu)16])2}, and {[Cu(hfac)2]([3-py-CH2CH2NH2(CH2)3SCH3][Cr7NiF8(O2CtBu)16])2}, the structures of which have been determined by X-ray diffraction. The {Cr7Ni} rings and CuII ions both have electronic spin S = 1/2, but with very different g-values. Continuous-wave EPR spectroscopy reveals the exchange interactions between these dissimilar spins, and hence the communication between the different molecular components that comprise these supramolecular systems. The interactions are weak such that we observe AX or AX2 type spectra. The connectivity between the {Cr7Ni} ring and thread terminus is varied such that the magnitude of the exchange interaction J can be tuned. The coupling is shown to be dominated by through-bond rather than through-space mechanisms.

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“…Furthermore, a rotaxane with pyridine as the stopper of the thread could be linked by a dinuclear copper cluster, [Cu 2 ( t BuCO 2 ) 4 ], to construct [3]rotaxanes (Figure 9 c). [31] Importantly, the heterometals may endow the metal–oxo ring with properties such as excellent redox, visible‐light absorption, and magnetic properties, which are important for potential applications of the host–guest systems in redox/photoresponsive devices and as quantum bits in quantum information processing [4, 18] …”

Section: The {Ti8o8} Cyclic Cluster For the Construction Of Molecularmentioning

confidence: 99%

Supramolecular Chemistry of Titanium Oxide Clusters

Liu

Wang

2021

Chemistry A European J

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Titanium oxide clusters (TOCs) have been emerging as a new type of inorganic molecular entities of supramolecular chemistry. Herein, a perspective on the structures and functionalities of TOCs over the past three decades is given and the paramount roles of TOCs in serving supramolecular chemistry are demonstrated. Four types of supramolecular assemblies based on TOCs are reviewed, namely, TOC hosts for ion inclusion, mechanically interlocked molecular systems built from cyclic TOCs, reactivities of surface sites toward ligand exchange, and hierarchical structures of TOCs. The principles and advantages of TOCs toward each application are fully discussed, along with structural analyses. Following this path, more functional TOC‐based supramolecular systems may be designed and synthesized in the future, which, in turn, will certainly enhance research into both supramolecular and coordination chemistry of titanium.

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Hybrid Organic–Inorganic Rotaxanes, Including a Hetero‐Hybrid [3]Rotaxane Featuring Two Distinct Heterometallic Rings and a Molecular Shuttle

Cited by 25 publications

References 25 publications

A [13]rotaxane assembled via a palladium molecular capsule

A [13]rotaxane assembled via a palladium molecular capsule

Close Encounters of the Weak Kind: Investigations of Electron–Electron Interactions between Dissimilar Spins in Hybrid Rotaxanes

Supramolecular Chemistry of Titanium Oxide Clusters

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