LAUSR

A robust single‐molecule light‐emitting diode (SM‐LED) with high color purity, linear polarization, and efficiency tunability is prepared by covalently integrating one fluorescent molecule into nanogapped graphene electrodes. Furthermore, single‐molecule Förster resonance energy transfer from the electroluminescent center to different accepters is achieved through rational molecular engineering, enabling construction of a multicolor SM‐LED. All these characterizations are accomplished in the photoelectrical integration system with high temporal/spatial/energy resolution, demonstrating the capability of the single‐photon emission of SM‐LEDs. The success in developing high‐performance SM‐LEDs inspires the development of the next generation of commercial display devices and promises a single‐photon emitter for use in quantum computation and quantum communication.