| Téléchargement | - Voir la version finale : Force spectroscopy of quadruple H-bonded dimers by AFM: dynamic bond rupture and molecular time−temperature superposition (PDF, 248 Kio)
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| DOI | Trouver le DOI : https://doi.org/10.1021/ja0531475 |
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| Auteur | Rechercher : Zou, Shan; Rechercher : Schönherr, Holger; Rechercher : Vancso, G. Julius |
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| Format | Texte, Article |
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| Résumé | We report on the application of the time−temperature superposition principle to supramolecular bond-rupture forces on the single-molecule level. The construction of force−loading rate master curves using atomic force microscopy (AFM)-based single-molecule force spectroscopy (SMFS) experiments carried out in situ at different temperatures allows one to extend the limited range of the experimentally accessible loading rates and hence to cross from thermodynamic nonequilibrium to quasi-equilibrium states. The approach is demonstrated for quadruple H-bonded ureido-4[1H]-pyrimidinone (UPy) moieties studied by variable-temperature SMFS in organic media. The unbinding forces of single quadruple H-bonding (UPy)₂ complexes, which were identified based on a polymeric spacer strategy, were found to depend on the loading rate in the range of 5 nN/s to 500 nN/s at 301 K in hexadecane. By contrast, these rupture forces were independent of the loading rate from 5 to 200 nN/s at 330 K. These results indicate that the unbinding behavior of individual supramolecular complexes can be directly probed under both thermodynamic nonequilibrium and quasi-equilibrium conditions. On the basis of the time−temperature superposition principle, a master curve was constructed for a reference temperature of 301 K, and the crossover force (from loading-rate independent to -dependent regimes) was determined as ∼145 pN (at a loading rate of ∼5.6 nN/s). This approach significantly broadens the accessible loading-rate range and hence provides access to fine details of potential energy landscape of supramolecular complexes based on SMFS experiments. |
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| Date de publication | 2005-08-01 |
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| Maison d’édition | American Chemical Society |
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| Dans | |
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| Langue | anglais |
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| Publications évaluées par des pairs | Oui |
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| Publication du CNRC | Cette publication n’est pas du CNRCCe sont des publications qui ont été rédigées par un auteur du CNRC, mais avant que celui-ci soit employé du CNRC. |
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| Exporter la notice | Exporter en format RIS |
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| Signaler une correction | Signaler une correction (s'ouvre dans un nouvel onglet) |
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| Identificateur de l’enregistrement | 10157f9b-403a-4e72-91fa-7925e8645f8c |
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| Enregistrement créé | 2019-04-15 |
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| Enregistrement modifié | 2020-05-30 |
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