Single-Molecule Detection of Acetylcholine by Translating the Neuronal Signal to a Single Distinct Electronic Peak

The bioelectric signal deriving from acetylcholine (ACh) plays an important role in regulating body function. Translating neuronal signals to electrical current peaks is a promising approach to achieve rapid detection of the bioelectric signal, but direct nanodevice-based single-molecule detection of the neurotransmitter is hampered by technology. Herein, we propose a neurotransmitter molecular nanogap device composed of atomically thin black phosphorus (BP) electrodes, which could rapidly distinguish the single distinct electronic peak of ACh at low positive bias from other central neurotransmitters. It is the first time that this unique electronic signal has been found, which originates from its quaternary ammonium group, and it has been experimentally verified in the linear sweep voltammetry (LSV) curves measured at 0.3 mV s^-1 in 0.01 M acetycholine chloride aqueous solution. Furthermore, our results suggest that replacing the N atom with a P atom can not only reverse the current signal but also change the signal magnitude in ACh or choline nanoelectronic devices. Importantly, all these appealing properties can even be assembled as components to make these molecules into parallel heterojunctions, making them a promising candidate for applications in forward or backward rectifying diodes. These results provide a theoretical basis for the creative applications of a BP electrode-based nanogap device in the rapid and single-molecule level detection of ACh, an electrochemical understanding for the mechanism of the signal transmission between neurons, and a physical approach to controlling the complex biological signal transduction in organisms. Ultimately, our findings lay the basis for next-generation biomedical solutions to clinical problems in the neurologic field.