The Shuttling Cascade in Lasso Peptide Benenodin-1 is Controlled by Non-Covalent Interactions |
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Authors: | Dr Hendrik V Schröder Dr Michael Stadlmeier Prof Martin Wühr Prof A James Link |
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Institution: | 1. Department of Chemical and Biological Engineering, Princeton University, Princeton, NJ, 08544 USA;2. Department of Molecular Biology and Lewis-Sigler Institute for Integrative Genomics, Princeton University, Princeton, NJ, 08544 USA |
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Abstract: | The lasso peptide benenodin-1, a naturally occurring and bacterially produced 1]rotaxane, undergoes a reversible zip tie-like motion under heat activation, in which a peptidic wheel stepwise translates along a molecular thread in a cascade of “tail/loop pulling” equilibria. Conformational and structural analyses of four translational isomers, in solution and in the gas phase, reveal that the equilibrium distribution is controlled by mechanical and non-covalent forces within the lasso peptide. Furthermore, each dynamic pulling step is accompanied by a major restructuring of the intramolecular hydrogen bonding network between wheel and thread, which affects the peptide's physico-chemical properties. |
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Keywords: | lasso peptides molecular switches natural products rotaxane supramolecular chemistry |
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