In this research, we explore sequence-dependent chiral-induced spin selectivity (CISS) in double-stranded (ds)-DNA using time-correlated single-photon counting and electrochemical impedance spectroscopy supplemented by tight-binding calculations of the phenomenon for the first time. The average lifetime of the photo-excited electrons in a Quantum Dot-DNA system is influenced by the CISS effect generated by the DNA molecule, and the difference in average time decay of electrons was found to be 345 ps for opposite polarity (“UP” and “DOWN”) of spins due to the CISS effect. Moreover, the yield of spin-polarized electrons due to the CISS effect was reduced by more than 35% from perfect DNA to DNA with point mutations. Remarkably, by employing a tight binding method combined with Green’s function formalism for transport, simulations of the process support the observed experimental trends. Our results provide a basic understanding of the sequence-specific spin-dependent electron transfer through ds-DNA. These results would help to build spin-based next-generation DNA sensors.

We design and build a novel light-amplified electrochemical impedimetric device based on the CISS effect to detect DNA hybridization using a hybrid quantum dot (QD)-DNA monolayer on a ferromagnetic (FM) Ni/Au thin film for the first time. Using spin as a detection tool, the current research considers the chiral-induced spin selectivity (CISS) phenomenon. After injecting a spin current into the QD-DNA system with opposite polarities (up and down), the impedimetric device revealed a large differential change in the charge-transfer resistance (ΔR ct ) of ∼100 ohms for both spins. Nearly, a threefold increase in the ΔR ct value to ∼270 ohms is observed when light with a wavelength of 532 nm is illuminated on the sample, owing to the amplified CISS effect. The yield of spin polarization as extracted from the Nyquist plot increases by a factor of more than 2 when exposed to light, going from 6% in the dark to 13% in the light. The impact of light on the CISS effect was further corroborated by the observation of the spin-dependent asymmetric quenching of photoluminescence (PL) in the same hybrid system. These observations are absent in the case of a noncomplementary QD-DNA system due to the absence of a helical structure in DNA. Based on this, we develop a spin-based DNA hybridization sensor and achieve a limit of detection of 10 fM. These findings open a practical path for the development of spin-based next-generation impedimetric DNA sensors and point-ofcare devices.