pH-Stimulated Concurrent Mechanical Activation of Two DNA “Tweezers”. A “SET−RESET” Logic Gate System

Abstract

A DNA tweezer consisting of C-rich arms is kept in the "closed" form by hybridization of the arms with a nucleic acid cross-linker. At acidic pH (pH = 5.2), the arms are stabilized through the formation of the i-motif, C-quadruplex structures, releasing the cross-linking nucleic acid and transforming the tweezer to its "opened" state. At neutral pH (pH = 7.2), the C-quadruplex structures are dissociated, resulting in the capturing of the cross-linking nucleic acid and the closure of the tweezer. By the reversible treatment of the tweezer at pH = 5.2 and at pH = 7.2, the tweezer system is cycled between the open and closed states, respectively, followed by a FRET process between a fluorophore-quencher pair that labels the tweezer. Also the concurrent activation of two DNA tweezers by pH stimuli is described. The pH-induced opening of one tweezer (tweezer A) by the formation of C-quadruplex (pH = 5.2) and the release of the cross-linking nucleic acid result in the closure of a second tweezer (tweezer B) by the hybridization of the released strand with the arms of tweezer B. The dissociation of the C-quadruplex structures (pH = 7.2) results in the favored translocation of the cross-linking nucleic acid from tweezer B to A. By the cycling of the pH of the system between pH = 5.2 and pH = 7.2, the concurrent opening and closure of the two tweezers are accomplished. The two tweezers system performs a SET-RESET logic gate operation, where the pH stimuli act as inputs.