Shrinking the size of photoelectrodes into the nanoscale will enable the precise modulation of cellular and subcellular behaviors of a single neuron and neural circuits. However, compared to photovoltaic devices, the reduced size causes the compromised efficiencies. Here, we present a highly efficient nanoelectrode based on bimetallic zinc and gold porphyrin (ZnAuPN). Upon light excitation, we observe ultrafast energy transfer (~66 ps) and charge transfer (~0.5 ps) through the porphyrin ring, enabling 97% efficiency in separating and transferring photoinduced charges to single Au-atom centers. Leveraging these isolated Au atoms as stimulating electrode arrays, we achieve significant photocurrent injection in single neurons, triggering action potential with millisecond light pulses. Notably, Extracranial near-infrared light irradiation of the motor cortex induces neuronal firing and enhances mouse movement. These results show the potential of nanoscale optoelectrodes for high spatiotemporal modulation of neuronal networks without the need for gene transfection in optogenetics.
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