Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology (KIT), D-76344 Eggenstein-Leopoldshafen, Germany.
Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), D-76344 Eggenstein-Leopoldshafen, Germany.
Phys Rev Lett. 2023 Jan 20;130(3):036201. doi: 10.1103/PhysRevLett.130.036201.
Electroluminescence from single molecules adsorbed on a conducting surface imposes conflicting demands for the molecule-electrode coupling. To conduct electrons, the molecular orbitals need to be hybridized with the electrodes. To emit light, they need to be decoupled from the electrodes to prevent fluorescence quenching. Here, we show that fully quenched 2,6-core-substituted naphthalene diimide derivative in a self-assembled monolayer directly deposited on a Au(111) surface can be activated with the tip of a scanning tunneling microscope to decouple the relevant frontier orbitals from the metallic substrate. In this way, individual molecules can be driven from a strongly hybridized state with quenched luminescence to a light-emitting state. The emission performance compares in terms of quantum efficiency, stability, and reproducibility to that of single molecules deposited on thin insulating layers. Quantum chemical calculations suggest that the emitted light originates from the singly charged cationic pair of the molecules.
吸附在导电表面上的单个分子的电致发光对分子-电极耦合提出了相互矛盾的要求。为了传导电子,分子轨道需要与电极杂化。为了发光,它们需要与电极解耦以防止荧光猝灭。在这里,我们表明,在 Au(111)表面上直接沉积的自组装单层中完全猝灭的 2,6-核取代萘二酰亚胺衍生物可以通过扫描隧道显微镜的尖端激活,以将相关的前沿轨道与金属基底解耦。通过这种方式,可以将单个分子从强杂交状态和猝灭的发光驱动到发光状态。就量子效率、稳定性和重现性而言,发光性能可与沉积在薄绝缘层上的单个分子相媲美。量子化学计算表明,发射光源自分子的单电荷阳离子对。