Light amplification by stimulated emission from an optically pumped molecular junction in a scanning tunneling microscope

Abstract: Here, we introduce and experimentally demonstrate optical amplification and stimulated emission from a single optically pumped molecular tunneling junction of a scanning tunneling microscope. The gap between a sharp gold tip and a flat gold substrate covered with a self-assembled monolayer of 5-chloro-2-mercaptobenzothiazole molecules forms an extremely small optical gain medium. When electrons tunnel from the molecules highest occupied molecular orbital to the tip, holes are left behind. These can be repopulated by hot electrons induced by the laser-driven plasmon oscillation on the metal surfaces enclosing the cavity. Solving the laser-rate equations for this system shows that the repopulation process can be efficiently stimulated by the gap modes near field, TERS scattering from neighboring molecules acting as an optical seed. Our results demonstrate how optical enhancement inside the plasmonic cavity can be further increased by a stronger localization via tunneling through molecules. We anticipate that stimulated emission from an STM junction will advance our fundamental understanding of quantum plasmonics and lead to new analytical applications. Furthermore, this concept represents the basis for novel ultra-small, fast, optically and electronically switchable devices and could find applications in high-speed signal processing and optical telecommunications.