Mechano-Electron Spin Coupling Modulates the Reactivity of Individual Coronazymes

Made of a nanozyme core covered with a DNAzyme corona, coronazyme exhibits superior peroxidase-like reactivity and selectivity. This can be attributed to the efficient transfer of the electrons generated at the nanozyme core to the DNA corona phase, demonstrating high substrate binding specificity. Leveraging magnetic-tweezer and highly inclined and laminated optical sheet (MT-HILO) microscopy, we discovered that the reactivity of the coronazyme is contingent upon the electron transfer efficiency governed by the sequence and architecture of the DNA corona. By applying tensile forces to disrupt this DNA, we observed a tenfold variation in reactivity within individual coronazymes. We found that the charge transfer in the coronazyme was modulated by altering electron spin polarization at the DNA-Au interface, which can be varied by a magnetic field or circularly polarized light (CPL), a hallmark for the chiral-induced spin selectivity (CISS) effect. Strikingly, we revealed that electron spin polarization was governed by the mechanical tension exerted on the DNA corona, demonstrating a hitherto unknown phenomenon of mechano-electron spin coupling.