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Controlling the structural transition between well-defined architectures found in living system is essential in polymer chemistry as well as material science. Herein, the reversible conformational switch of a non-natural polypeptide with an aromatic ring (2,6-naphthalene spacer) on its peptide backbone, referred to as an arylopeptide, between two distinct well-defined helical structures (extended 31 -helix and contracted 41 -helix) using side chain solvation is demonstrated. The folding selectivity of the arylopeptide and found that the
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